bluuebunny/crossref_metadata_2025 huggingface dataset:
A Multifunctional Cobalt‐Containing Implant for Treating Biofilm Infections and Promoting Osteointegration in Infected Bone Defects Through Macrophage‐Mediated Immunomodulation
Authors: Yan Nongyang , Zhou Hao , Jin Penghe , Li Tengfei , Liu Qi , Ning Hao , Ma Zhixin , Feng Linfei , Jin Tao , Deng Youwen , Wu Zhengwei
Published: November 2024

Treating bone infections and ensuring bone recovery is one of the major global problems facing modern orthopedics. Prolonged antibiotic use may increase the risk of antimicrobial resistance, and inflammation caused by biofilms can obstruct tissue healing, making bone infection treatment even more challenging. The optimal treatment strategy combines immune response modification to promote osteogenesis with effective bacterial infection removal that does not require long‐term antibiotic use. A one‐step plasma immersion ion implantation approach is used to create titanium alloy implants incorporating cobalt. According to experimental findings, cobalt‐containing titanium implants exhibit improved antibacterial activity by efficiently disrupting biofilm formations and reducing Methicillin‐resistant Staphylococcus aureus adherence by over 80%. Additionally, the implants exhibit superior anti‐inflammatory and osseointegration properties. RNA sequencing analysis reveals the potential mechanism of Co2+ in regulating the polarization of macrophages toward the anti‐inflammatory M2 phenotype, which is crucial for creating an immune environment conducive to bone healing. Concurrently, these implants promote osteogenic differentiation while suppressing osteoclast activity, further supporting bone repair. Overall, without exogenous recombinant proteins or antibiotics, the implants effectively eradicate infections and expedite bone repair, offering a novel therapeutic strategy for complex skeletal diseases with clinical promise.
Multi‐Mechanism Collaborative Bionic Fixation Technique Between a Wide Range of Solid Interfaces
Authors: Fu Shixun , Sun Jun , Hu Zhiyong , Zhao Yongjin , Yao Tianchang , Wang Xipeng , Ji Yuanming , Deng Kai , Ji Keju
Published: November 2024

For rough surfaces, stable, fast, and repeatable fixation has wide applicability in transportation, fire protection, and other fields. Different rough surfaces present technical challenges for achieving convenient and reliable fixation. Based on the highly adhesive attachment structures of typical organisms, a multi‐mechanism (negative pressure adsorption, mechanical locking, and chemical bonding) cooperative bionic fixation device is proposed. The device is equipped with a suction disc with gradient guide channels, a microneedles friction‐enhancing unit, and fast‐curable UV glue. These components work together to complete the fixation. The detachment work (max. 5.7 and 5.5 J) and pull‐off force (max. 377 and 175 N) are evaluated on sandpaper of different roughness under vertical and horizontal pulling respectively. By analyzing the detachment process and experimental curves, the cooperative principle of the multi‐mechanism is identified. In addition, the microneedles with soft backing at the bionic fixation device bottom improve its adaptability to rough surfaces. The gradient guide channels of the suction disc create Laplace pressure to speed up the UV glue flow and shorten fixation time. Furthermore, its applicability is demonstrated by combining it with monitoring equipment and an adult to attach to rough surfaces.
Using the Transversal Admittance to Understand Organic Electrochemical Transistors
Authors: Bisquert Juan , Keene Scott T.
Published: November 2024

The transient behavior of organic electrochemical transistors (OECTs) is complex due to mixed ionic‐electronic properties that play a central role in bioelectronics and neuromorphic applications. Some works applied impedance spectroscopy in OECTs for understanding transport properties and the frequency‐dependent response of devices. The transversal admittance (drain current vs gate voltage) is used for sensing applications. However, a general theory of the transversal admittance, until now, has been incomplete. The derive a model that combines electronic motion along the channel and vertical ion diffusion by insertion from the electrolyte, depending on several features as the chemical capacitance, the diffusion coefficient of ions, and the electronic mobility. Based on transport and charge conservation equations, it is shown that the vertical impedance produces a standard result of diffusion in intercalation systems, while the transversal impedance contains the electronic parameters of hole accumulation and transport along the channel. The spectral shapes of drain and gate currents and the complex admittance spectra are established by reference to equivalent circuit models for the vertical and transversal impedances, that describe well the measurements of a PEDOT:PSS OECT. New insights are provided to the determination of mobility by the ratio between drain and gate currents.
Sequentially Activated Smart DNA Nanospheres for Photoimmunotherapy and Immune Checkpoint Blockade
Authors: Chen Yu , Guo Yu , Cheng Wen , Fan Jiahao , Li Jiacheng , Song Jiajia , Yang Xiaohai , Wang Kemin , Huang Jin
Published: November 2024

Due to the inherent immunosuppression and immune evasion of cancer cells, combining photoimmunotherapy with immune checkpoint blockade leverages phototherapy and immune enhancement, overcoming mutual limitations and demonstrating significant anticancer potential. The main challenges include nonspecific accumulation of agents, uncontrolled activation, and drug carrier safety. Smart DNA nanospheres (NS) is developed with targeted delivery and controllable release of photosensitizers and immune agents to achieve effective synergistic therapy and minimize side effects. The multifunctional NS incorporate a targeting module for programming aptamers, a response module for programming i‐motif and DNA/RNA hybrid sequences, and a therapeutic module for packaging photosensitizers and PD‐L1 siRNA. NS navigate to the tumor site and are sequentially activated by intracellular acid and enzymes to release photosensitizers and programmed death ligand 1 (PD‐L1) small interfering RNA (siRNA). Besides tumor killing and immune promotion, activated NS downregulate PD‐L1 expression, alleviating immune tolerance and evasion, thus enhancing the immune response. These results indicate that NS significantly enhance antitumor immune responses, synergistically improve antitumor efficacy, and reduce systemic toxicity. This study broadens the application of DNA nanomaterials in precision drug delivery and tumor therapy.
Oxygen‐Doped 2D In2Se3 Nanosheets with Extended In‐Plane Lattice Strain for Highly Efficient Piezoelectric Energy Harvesting
Authors: Kim Ji Yeon , Hwang Woohyun , Han Seo Yeon , Jung Ye Seul , Pang Fengyi , Shen Wenhu , Park Cheolmin , Kim Sang‐Woo , Soon Aloysius , Cho Yong Soo
Published: November 2024

With the emergence of electromechanical devices, considerable efforts have been devoted to improving the piezoelectricity of 2D materials. Herein, an anion‐doping approach is proposed as an effective way to enhance the piezoelectricity of α‐In2Se3 nanosheets, which has a rare asymmetric structure in both the in‐plane and out‐of‐plane directions. As the O2 plasma treatment gradually substitutes selenium with oxygen, it changes the crystal structure, creating a larger lattice distortion and, thus, an extended dipole moment. Prior to the O2 treatment, the lattice extension is deliberately maximized in the lateral direction by imposing in situ tensile strain during the exfoliation process for preparing the nanosheets. Combining doping and strain engineering substantially enhances the piezoelectric coefficient and electromechanical energy conversion. As a result, the optimal harvester with a 0.9% in situ strain and 10 min plasma exposure achieves the highest piezoelectric energy harvesting values of ≈13.5 nA and ≈420 µW cm−2 under bending operation, outperforming all previously reported 2D materials. Theoretical estimation of the structural changes and polarization with gradual oxygen substitution supports the observed dependence of the electromechanical performance.
Magnetic Field Screening of 2D Materials Revealed by Magnetic Force Microscopy
Authors: Aldave Diego A. , López‐Polín Guillermo , Calle Esther , Begué Adrián , Ranchal Rocío , Martínez Raúl , Bran Cristina , Burzurí Enrique , Gómez‐Herrero Julio , Ares Pablo , Jaafar Miriam
Published: November 2024

2D materials possess exceptional mechanical properties making them promising candidates for protecting nanostructures. However, the magnetic field screening properties of 2D materials are largely unexplored. Here it is used Magnetic Force Microscopy (MFM) to unveil the effects on the magnetic field of magnetic nanostructures when 2D materials are placed on top of them. It is demonstrated that while graphene exhibits a weak diamagnetic response due to its unique electronic structure around the Dirac point, the overall screening effect remains minimal (≈0.5% per layer). Conversely, graphene oxide (GO) and MoS2 show negligible response to the magnetic field, making them ideal for applications where preserving the original magnetic properties is crucial. These findings suggest that 2D materials can offer effective protection while minimally affecting the underlying magnetic functionalities, important for data storage technologies and spintronics.
Simultaneous optimization of simulated moving bed adsorption and distillation for 2,3‐butanediol recovery
Authors: Avendano Marco , Fu Qiang , Lao Jianpei , Nair Sankar , Realff Matthew J.
Published: November 2024

A combined simulated moving bed (SMB) and distillation separation scheme is developed to recover 2,3‐butanediol (BDO) from a dilute fermentation broth. The scheme was integrated into a lignocellulosic biorefinery that produces hydrocarbon fuels from corn stover with BDO as an intermediate. BDO recovery is one of the most challenging processes in this biorefinery; and given the high associated energy duties, direct distillation is considered cost‐prohibitive. An alternative separation is SMB adsorption in nanoporous materials, which can reject 90% of the water and reduce subsequent distillation costs. Rigorous models were used to optimize the SMB and distillation simultaneously. The separation can be added to the biorefinery while keeping the projected minimum fuel selling price (MFSP) below $0.66 USD (US dollars) per liter gasoline‐equivalent ($2.50/GGE, gallon gasoline equivalent). Finally, sensitivity analyses were conducted to assess the effects of cost and lifetime of the adsorbent, titer concentration, and BDO purity.
Ecofriendly Printed Wood‐Based Honey‐Gated Transistors for Artificial Synapse Emulation
Authors: Vieira Douglas Henrique , Carlos Emanuel , Ozório Maíza Silva , Morais Maria , Fortunato Elvira , Alves Neri , Martins Rodrigo
Published: November 2024

Printed electronics have traditionally used substrates and materials derived from fuel‐based or less abundant and toxic resources, raising environmental concerns. Wood as a substrate reduces processing steps and enables the integration of intelligent functionalities in wooden furniture, offering biodegradability, nontoxicity, and derivation from renewable sources. In this work, sustainably printed transistors using zinc oxide nanoparticles as the active layer and honey electrolyte on wood substrates are demonstrated as a promising approach to reduce the environmental footprint of electronics. Despite the substrate's high roughness, the transistor exhibits excellent performance for screen‐printed devices, with low on‐voltage of 0.32 ± 0.12 V and high Ion/Ioff of (2.4 ± 0.9) × 104. Further analysis of hysteresis in transfer curves under varying scan rates and sweep ranges reveals the device's ability to adjust memory windows and on‐current. Notably, these devices successfully emulate synapses, exhibiting neural facilitation and plasticity, indicating a shift toward sustainable computing. The device's dynamic response to single and successive presynaptic pulses demonstrates its ability to adjust synaptic weight, transition from transient to persistent memory, and pulse width‐, frequency‐, voltage‐, and number‐dependent excitatory postsynaptic currents. The successful emulation of the learning–forgetting–relearning–forgetting process underscores the device's potential for use in sustainable high‐performance neuromorphic systems.
NaI‐promoted Synthesis of 2‐aryl Benzothiazole/Benzoxazole in Aqueous Medium
Authors: Lian Zhongwenqin , Ge Xin , Chen Hejun , Wusiman Mukerimu , Ablajan Keyume
Published: November 2024

A NaI‐promoted efficient synthesis of 2‐aryl benzothiazoles/benzoxazoles with various substituted acyl chlorides is described. The reaction proceeded using more environment‐friendly H2O media as a solvent. Mechanism studies verified that the reaction undergoes a ring‐opening process. This novel method could be suitable for benzothiazole and benzoxazole to afford good yields of arylated products. This protocol has the potential for further application due to its broad substrate scopes.
Helical π‐Extended Terrylene Diimide Dimer Based on Ring‐Fused Ethylene Bridge for Organic Solar Cells
Authors: Dai Luyao , Shao Guangwei , You Xiaoxiao , Chen Li , Wu Di , Xia Jianlong
Published: November 2024

Terrylene diimides (TDIs), as the higher homologues of perylene diimide (PDI) in the series of rylene diimides (RDIs), exhibit several especial properties including enhanced absorption ability in the near infrared (NIR) region, higher fluorescence quantum yields as well as stronger π–π stacking in comparison to naphthalene diimides (NDIs) and perylene diimides (PDIs). However, TDIs have been largely overlooked in terms of their photovoltaic applications because of the chemical inaccessibility and poor solubility. In this contribution, a helical π‐extended terrylene diimide dimer based on ring‐fused ethylene bridge, namely FTDI2 is designed and synthesized. The photovoltaic performances of FTDI2 and the parent TDI are investigated using the commercially available PTB7‐Th as the electron donor. A significantly improved power‐conversion efficiency (PCE) of 5.11 % compared to that of TDI based ones (0.5 %) is achieved for FTDI2‐based device, demonstrating the potential of terrylene dyes in the photovoltaics field.
Communication Bridge‐2 randomized controlled trial: Recruitment and baseline features
Authors: Rogalski Emily , Bona Matthew , Esparza Marissa , Mooney Aimee , Fried‐Oken Melanie , Rademaker Alfred , Roberts Angela
Published: November 2024

INTRODUCTION

Non‐pharmacological interventions may offer significant benefits to the quality of life for persons with primary progressive aphasia (PPA) and their care partners but have lacked efficacy trials. To help fill the efficacy gap, we provide the feasibility of recruitment, enrollment, randomization, and baseline data for the Communication Bridge‐2 (CB2) randomized controlled trial (RCT).

METHODS

CB2 is the first international, single enrollment site, Phase 2, Stage 2, parallel‐group, active control, RCT delivered via video chat to individuals with PPA and their care partners. Participants were recruited, screened, and randomized into one of two speech–language intervention arms.

RESULTS

Ninety‐five participant dyads (PPA mean baseline age: 67.1; 48% female) from four countries were enrolled and randomized.

DISCUSSION

Global recruitment, enrollment, and randomization of individuals with PPA into a video chat–delivered non‐pharmacologic RCT is feasible. This trial provides a potential model for conducting rigorous non‐pharmacologic efficacy trials for Alzheimer's disease and related dementias.

Highlights

Primary progressive aphasia (PPA) negatively impacts communication participation.

Communication Bridge‐2 (CB2) is a telemedicine‐delivered randomized controlled trial.

CB2 included global recruitment and randomization of 95 PPA participant dyads.

CB2, the first international superiority trial for PPA using video chat shows feasibility.

The study provides a model for rigorous non‐pharmacologic trials for Alzheimer's disease and related dementias.
Heritability of Alzheimer's disease plasma biomarkers: A nuclear twin family design
Authors: Rousset Rebecca Z. , den Braber Anouk , Verberk Inge M. W. , Boonkamp Lynn , Wilson David H. , Ligthart Lannie , Teunissen Charlotte E. , de Geus Eco J. C.
Published: November 2024

INTRODUCTION

Alzheimer's disease (AD) is a highly heritable disease (60%–80%). Amyloid beta (Aβ) 42/40, neurofilament light chain (NfL), and glial fibrillary acidic protein (GFAP) are plasma biomarkers for AD. Clinical biomarker research would be served by an understanding of the sources of variance in these markers.

METHODS

Blood concentrations of Aβ42/40, NfL, and GFAP of twins and their families (monozygotic twins: 1574, dizygotic twins: 1266, other: 3657) were analyzed on the Simoa HD‐X. Twin‐family models were used to estimate proportional genetic contributions to the variance in biomarker levels.

RESULTS

Heritability estimates were 16% for Aβ42/40, 42% for NfL, and 60% for GFAP. NfL and GFAP were significantly correlated with each other (0.37) but not with Aβ42/40.

DISCUSSION

The heritability of Aβ42/40 (16%) is lower than the heritability of AD, suggesting strong environmental influences on this biomarker. The lack of correlation between NfL/GFAP and Aβ42/40 indicates these markers may be on different biological pathways.

Highlights

Heritability is found for glial fibrillary acidic protein (60%), neurofilament light chain (42%), and amyloid beta (Aβ) 42/40 (16%) plasma levels.

Aβ42/40 plasma levels are sensitive to person‐specific environmental influences.
Increased Disability Progression in rs10191329AA Carriers with Multiple Sclerosis Is Preceded by Neurofilament Light Chain Elevations
Authors: Protopapa Maria , Steffen Falk , Schraad Muriel , Ruck Tobias , Öztürk Menekse , Hanuscheck Nicholas , Shin Josef , Brummer Tobias , Pape Katrin , Uphaus Timo , Meuth Sven G. , Fleischer Vinzenz , Teunissen Charlotte E. , De Jager Philip L. , Luessi Felix , Bittner Stefan , Zipp Frauke
Published: November 2024

Objective

We examined the impact of the rs10191329 genetic risk variant on neuroaxonal damage as measured by serum neurofilament light chain (sNfL) levels, and disability progression in people with multiple sclerosis (pwMS).

Methods

In a cohort of pwMS (n = 740), 658 participants were prospectively monitored every 2 years for less than a decade while 82 of 740 pwMS were monitored retrospectively for up to 40 years. We investigated associations between rs10191329 variants and clinical outcome, including Expanded Disability Status Scale (EDSS), disability accrual (defined by EDSS‐increase of at least 1.5 for patients starting at EDSS 0, at least 1.0 EDSS‐points for patients with an initial EDSS between 1 and 4.5 and at least 0.5 points for patients starting with an EDSS equal or greater than 5) and progression to secondary progressive MS (SPMS). Clinical outcomes were analyzed using Kaplan–Meier and Cox proportional hazards analyses. Disability accumulation over time was depicted using a generalized mixed‐effect model. Single‐molecule array was used to assess sNfL levels.

Results

Homozygous, heterozygous, and non‐carriers of the rs10191329 risk variant displayed comparable sNfL levels indicating similar neuroaxonal damage at the time of diagnosis. Importantly, in homozygous carriers we found highest sNfL levels in follow‐up visits preceding elevated disease progression later in the disease course, a steeper increase in overall disability measures and higher probability of SPMS development.

Interpretation

These findings highlight how genetic variants may serve as new biomarkers for disease progression and can be used for personalized medicine and risk assessment in MS. ANN NEUROL 2025;97:596–605
Skelettale Stickstoff‐Funktionalisierung von isostrukturellen 2D‐konjugierten MOFs zur Verbesserung der Doppelionen Speicherkapazität
Authors: Sporrer Lukas , Guo Quanquan , Li Xiaodong , Wrzesinska‐Lashkova Angelika , Reichmayr Fanny , Fu Shuai , Wang Hai I. , Bonn Mischa , Li Xiangyu , Laval‐Schmidt Paul‐Alexander , Wang Mingchao , Lu Yang , Vaynzof Yana , Yu Minghao , Feng Xinliang , Dong Renhao
Published: November 2024

Zweidimensionale konjugierte metallorganische Gerüste (2D c‐MOFs) kommen als vielversprechende Elektrodenmaterialien für elektrochemische Energiespeicherung auf. Eine einfache Methode zur Realisierung verbesserter Doppelionen Speicherung in 2D c‐MOFs ist jedoch nicht bekannt. Hier berichten wir über die Synthese von Cu2(Nx−OHPTP) 2D c‐MOFs (x=0,1,2; OHPTP=Octahydroxyphenanthrotriphenylen) mit ein oder zwei präzisen aromatischen Kohlenstoff‐Stickstoff‐Ersetzungen im π‐konjugierten OHPTP‐Liganden. Die Stickstoff‐Modifikation des aromatischen Skeletts in Cu2(Nx−OHPTP) ermöglicht die synergistische Einführung zusätzlicher Redoxstellen und begünstigt damit wesentlich die Doppelionen Adsorptionskapazität. Folglich zeigt die Cu2(N2−OHPTP) Kathode eine stark verbesserte elektrochemische Leistung bei der Speicherung von zwei Ionen (d. h. Li+ und Cl‐) mit einer hohen spezifischen Kapazität von 53.8 mAh g−1. Diese ist doppelt so hoch wie die von Cu2(N0−OHPTP) und 1.3 mal so hoch wie die von Cu2(N1−OHPTP). Darüber hinaus zeigt die Cu2(N2−OHPTP) Elektrode eine günstige Ratenleistung von 52 % und eine gute Stabilität von 96 % der initialen Kapazität nach 1000 Zyklen. Durch die Kombination von ex situ‐ und in situ Spektroskopie Messungen und theoretischen Berechnungen identifizieren wir N‐Redoxpositionen als zusätzliche Li+‐Adsorptionsorte. Darüber hinaus unterstreichen Berechnungen die synergistische Erhöhung der Cl− Adsorptionsenergie um etwa 1.0 eV an den elektronenärmeren CuO4‐Verknüpfungen welche durch N‐Inkorporation verursacht wird. Diese Arbeit ebnet den Weg zum präzisen Design von 2D c‐MOFs mit verbesserten elektrochemischen Eigenschaften und erweitert deren Anwendung in der Doppelionen Speicherung.
Ce3+/Ce4+ Ion Redox Shuttle Stabilized Cuδ+ for Efficient CO2 Electroreduction to C2H4
Authors: Liu Xiang , Liu Ting , Ouyang Ting , Deng Jiguang , Liu Zhao‐Qing
Published: November 2024

The CO2 electroreduction reaction has advantages in clean and pollution‐free carbon conversion, but it still faces challenges in carbon utilization efficiency and improving the selectivity of C2 products. Although the dynamic Cuδ+ state is known to favor the C−C coupling process, the suitable Cuδ+ species for electrocatalytic reduction of CO2 are difficult to maintain under the conditions of strong reduction and large current. Herein, we propose a Ce doping strategy to stabilize the Cuδ+ state (Ce/CuOx) during the CO2RR process, which enables a high Faradaic efficiency of 60 % for multi‐carbon products (40 % for C2H4, 14 % for CH3CH2OH, and 6 % for CH3COOH), and 25 h stability at −1.2 V versus the reversible hydrogen electrode. In situ infrared spectroscopy, in situ X‐ray photoelectron spectroscopy combined with density functional theory calculations reveal that the Cuδ+ is stabilized by the redox ion pairs of Ce, which reduces the energy barrier of *CO coupling, and improves the Faraday efficiency of electrocatalytic CO2 reduction of C2H4. This work provides a new idea to make full use of lanthanide variable value metals for advanced catalysis and clean energy conversion.
Hollow Pt‐Encrusted RuCu Nanocages Optimizing OH Adsorption for Efficient Hydrogen Oxidation Electrocatalysis
Authors: Wei Licheng , Dong Yuanting , Yan Wei , Zhang Yuqi , Zhan Changhong , Huang Wei‐Hsiang , Pao Chih‐Wen , Hu Zhiwei , Lin Haixin , Xu Yong , Geng Hongbo , Huang Xiaoqing
Published: November 2024

As one of the best candidates for hydrogen oxidation reaction (HOR), ruthenium (Ru) has attracted significant attention for anion exchange membrane fuel cells (AEMFCs), although it suffers from sluggish kinetics under alkaline conditions due to its strong hydroxide affinity. In this work, we develop ternary hollow nanocages with Pt epitaxy on RuCu (Pt‐RuCu NCs) as efficient HOR catalysts for application in AEMFCs. Experimental characterizations and theoretical calculations confirm that the synergy in optimized Pt8.7‐RuCu NCs significantly modifies the electronic structure and coordination environment of Ru, thereby balancing the binding strengths of H* and OH* species, which leads to a markedly enhanced HOR performance. Specifically, the optimized Pt8.7‐RuCu NCs/C achieves a mass activity of 5.91 A mgPt+Ru−1, which is ~3.3, ~2.2, and ~15.0 times higher than that of RuCu NCs/C (1.38 A mgRu−1), PtRu/C (1.83 A mgPt+Ru−1) and Pt/C (0.37 A mgPt−1), respectively. Impressively, the specific peak power density of fuel cells reaches 15.9 W mgPt+Ru−1, significantly higher than those of most reported PtRu‐based fuel cells.
Rational Molecular Design for Balanced Locally Excited and Charge‐ Transfer Nature for Two‐Photon Absorption Phenomenon and Highly Efficient TADF‐Based OLEDs
Authors: Mageswari Gomathi Vinayakam , Chitose Youhei , Tsuchiya Youichi , Lin Ja‐Hon , Adachi Chihaya
Published: November 2024

The pursuit of highly efficient thermally activated delayed fluorescence (TADF) emitters with two‐photon absorption (2PA) character is hampered by the concurrent achievement of a small singlet‐triplet energy gap (ΔEST) and high photoluminescence quantum yield (ΦPL). Here, by introducing a terephthalonitrile unit into a sterically crowded donor‐π‐donor structure, inducing a hybrid electronic excitation character, we designed unique TADF emitters possessing 2PA ability. This rational molecular design was achieved through a main π‐conjugated donor‐acceptor‐donor backbone in line with locally excited feature renders a large oscillator strength and transition dipole moment, maintaining a high 2PA cross‐section value. The ancillary N‐donor‐acceptor‐donor with charge transfer character highly balances the TADF phenomenon by minimizing ΔEST. A near‐unity ΦPL value with a large radiative decay rate over an order of magnitude higher than the intersystem crossing rate and a high horizontal orientation ratio of 0.95 were simultaneously attained for TPCz2NP. The organic light‐emitting diodes fabricated with this material exhibit a high maximum external quantum efficiency of 25.4 % with an elevated 2PA cross‐section (σ2) value up to 143 GM at 850 nm. These findings offer a venue for designing high‐performance TADF emitters with exceptional performance inclusive of 2PA properties, expanding for future functional material design.
Unconventional Heterobidentate Coordination of 4‐Hydroxypyridine Leading to Remarkably Strong Second‐Harmonic Generation in Zn(C5H4NO)2
Authors: Yang Can , Gou Jie , Zhu Yaolong , Xiong Yi , Zhu Zece , Chen Ling , Wu Qi
Published: November 2024

Herein, we report an unconventional heterobidentate coordination mode of conventional 4‐hydroxypyridine ligand in a novel compound Zn(C5H4NO)2. The strong heterobidentate coordination interactions between Zn2+ and 4‐hydroxypyridine ligands promote a uniform alignment of the polarization of each [ZnO2N2] tetrahedral building unit, resulting in remarkably strong second‐harmonic generation (SHG) with an intensity that is the largest among all UV‐transparent Zn‐containing metal‐organic compounds reaching 13.6×KDP. Moreover, Zn(C5H4NO)2 processes a suitable optical band gap of 4.40 eV, high thermal stability up to 300 °C, excellent air stability, and strong water resistance, demonstrating great application potential. Additionally, Zn(C5H4NO)2 exhibits photoluminescence with a significantly enhanced lifetime of 558 ms, accompanied by a rare blue afterglow visible to the naked eye, lasting up to 5 s.
Near‐Infrared Chemiluminophore Switches Photodynamic Processes via Protein Complexation for Biomarker‐Activatable Cancer Therapy
Authors: Huang Jingsheng , Liu Jing , Wu Jiayan , Xu Mengke , Lin Youshi , Pu Kanyi
Published: November 2024

Despite the potential in cancer therapy, phototheranostic agents often face two challenges: limited diagnostic sensitivity due to tissue autofluorescence and suboptimal therapeutic efficacy due to the Type‐II photodynamic process with the heavy oxygen reliance. In contrast, chemiluminescent theranostic agents without the requirement of real‐time light excitation can address the issue of tissue autofluorescence, which however have been rarely reported for photodynamic therapy (PDT), not to mention less oxygen‐dependent Type‐I PDT. In this work, we synthesize near‐infrared (NIR) chemiluminophores with the specific binding towards human serum albumin (HSA) to form chemiluminophore‐protein complex for cancer detection and photodynamic therapy. Interestingly, after the complexation with HSA, the chemiluminescence (CL) intensities of chemiluminophores are enhanced by over 10‐fold; meanwhile, the photodynamic process switches from Type‐II (singlet‐oxygen‐generation dominated) to Type‐I (superoxide anion and hydroxyl radical dominated), while the previously reported activated chemiluminophore with non‐specific HSA binding can't switch photodynamic process. Based on the optimal chemiluminophore, a nitroreductase‐activatable CL probe‐protein complex is synthesized, which specially turns on its CL and Type‐I PDT in hypoxic tumors for precision therapy. Thus, this study provides a complexation strategy to improve phototheranostic performance of chemiluminophores.
Organic Molecule Functionalization Enables Selective Electrochemical Reduction of Dilute CO2 Feedstock
Authors: Wang Bingqing , Wang Xingyu , Wu Bo , Li Peize , Chen Shenghua , Lu Ruihu , Lai Weifei , Shen Yan , Zhuang Zechao , Zhu Jiexin , Wang Ziyun , Wang Dingsheng , Lum Yanwei
Published: November 2024

The electrochemical conversion of low‐concentration CO2 feedstock to value‐added chemicals and fuels is a promising pathway for achieving direct valorization of waste gas streams. However, this is challenging due to significant competition from the hydrogen evolution reaction (HER) and lowered CO2 reduction (CO2R) kinetics as compared to systems that employ pure CO2. Here we show that terephthalic acid (TPA) functionalization can boost selectivity towards CO2R and suppress HER over a range of catalysts including Bi, Cu and Zn. For instance, TPA functionalized Bi attained a formate Faradaic efficiency (FEHCOO‐) of 96.3 % at 300 mA cm−2 with pure CO2 feedstock. Density functional theory simulations indicate that this is because TPA functionalization modulates the binding energies of the key reaction intermediates *OCHO and *H. With low‐concentration feedstock (15 % CO2) at 100 mA cm−2, we achieved a high FEHCOO‐ of 85.8 %, which was double that of an unmodified Bi catalyst. Using an electrolyzer with a porous solid electrolyte layer, we successfully showcase 30 h of continuous high‐purity formic acid production with a 5 % CO2 feed. Taken together, our findings demonstrate that molecular tuning of a catalyst can be an effective strategy for enabling selective CO2R using low‐concentration feedstock.
Cooperative Active Sites on Ag2Pt3TiS6 for Enhanced Low‐Temperature Ammonia Fuel Cell Electrocatalysis
Authors: Wu Tong , Dhaka Kapil , Luo Mengjia , Wang Bingqing , Wang Meng , Xi Shibo , Zhang Mingsheng , Huang Fuqiang , Exner Kai S. , Lum Yanwei
Published: November 2024

Ammonia has attracted considerable interest as a hydrogen carrier that can help decarbonize global energy networks. Key to realizing this is the development of low temperature ammonia fuel cells for the on‐demand generation of electricity. However, the efficiency of such systems is significantly impaired by the sluggish ammonia oxidation reaction (AOR) and oxygen reduction reaction (ORR). Here, we report the design of a bifunctional Ag2Pt3TiS6 electrocatalyst that facilitates both reactions at mass activities exceeding that of commercial Pt/C. Through comprehensive density functional theory calculations, we identify that active site motifs composed of Pt and Ti atoms work cooperatively to catalyze ORR and AOR. Notably, in situ shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) experiments indicate a decreased propensity for *NOx formation and hence an increased resistance toward catalyst poisoning for AOR. Employing Ag2Pt3TiS6 as both the cathode and anode, we constructed a low temperature ammonia fuel cell with a high peak power density of 8.71 mW cm−2 and low Pt loading of 0.45 mg cm−2. Our findings demonstrate a pathway towards the rational design of effective electrocatalysts with multi‐element active sites that work cooperatively.
Optically Modulated Nanofluidic Ionic Transistor for Neuromorphic Functions
Authors: Wang Jiao , Jiang Yanan , Xiong Tianyi , Lu Jiahao , He Xiulan , Yu Ping , Mao Lanqun
Published: November 2024

Neuromorphic systems that can emulate the behavior of neurons have garnered increasing interest across interdisciplinary fields due to their potential applications in neuromorphic computing, artificial intelligence and brain‐machine interfaces. However, the optical modulation of nanofluidic ion transport for neuromorphic functions has been scarcely reported. Herein, inspired by biological systems that rely on ions as signal carriers for information perception and processing, we present a nanofluidic transistor based on a metal–organic framework membrane (MOFM) with optically modulated ion transport properties, which can mimic the functions of biological synapses. Through the dynamic modulation of synaptic weight, we successfully replicate intricate learning‐experience behaviors and Pavlovian associate learning processes by employing sequential optical stimuli. Additionally, we demonstrate the application of the International Morse Code with the nanofluidic device using patterned optical pulse signals, showing its encoding and decoding capabilities in information processing process. This study would largely advance the development of nanofluidic neuromorphic devices for biomimetic iontronics integrated with sensing, memory and computing functions.
Versatile Strategy for the Chemoenzymatic Synthesis of Branched Human Milk Oligosaccharides Containing the Lacto‐N‐Biose Motif
Authors: Tseng Hsin‐Kai , Lee Ting‐Yi , Chiang Yu‐Ching , Kuo Wen‐Hua , Tseng Hsien‐Wei , Wang Hung‐Kai , Ni Chi‐Kung , Lin Chun‐Cheng
Published: November 2024

Human milk oligosaccharides (HMOs) exhibit prebiotic, antimicrobial, and immunomodulatory properties and confer significant benefits to infants. Branched HMOs are constructed through diverse glycosidic linkages and prominently feature the lacto‐N‐biose (LNB, Gal‐β1,3‐GlcNAc) motif with fucose and/or sialic acid modifications, displaying structural complexity that surpasses that of N‐ and O‐glycans. However, synthesizing comprehensive libraries of branched HMO is challenging due to this complexity. Although a few systematic synthetic strategies have emerged, many of them rely on labor‐intensive chemical methodologies or exploit the substrate specificity of human N‐acetylglucosaminyltransferase 2 (hGCNT2). In this study, we capitalized on the substrate promiscuities of hGCNT2 and bacterial glycosyltransferases (GTs) to construct a universal tetrasaccharide core in a highly efficient manner. This core was systematically and flexibly extended to generate diverse branched HMOs utilizing the promiscuity of bacterial GTs coupled with N‐trifluoroacetyl glucosamine (GlcNTFA), which facilitated sugar chain elongation. The GlcNTFA residues were subsequently converted into various N‐modified glucosamines through straightforward chemical manipulations to modulate the activities of additional GTs during glycan extension. These masked amino groups were ultimately reverted to N‐acetyl groups, facilitating the synthesis of a broad range of asymmetric and multiantennary HMOs featuring LNB moieties, including many previously inaccessible structures.
Dual Regulation of Sensitizers and Cluster Catalysts in Metal–Organic Frameworks to Boost H2 Evolution
Authors: Guo Song , Pan Chun‐Wei , Hou Min , Hou Yi‐Tong , Yao Shuang , Lu Tong‐Bu , Zhang Zhi‐Ming
Published: November 2024

Photocatalytic efficiency is closely correlated to visible‐light absorption ability, electron transfer efficiency and catalytic center activity of photocatalysts, nevertheless, the concurrent management of these factors to improve photocatalytic efficiency remains underexplored. Herein, we proposed a sensitizer/catalyst dual regulation strategy on the polyoxometalate@Metal−Organic Framework (POM@MOF) molecular platform to construct highly efficient photocatalysts. Impressively, Ni−Sb9@UiO−Ir−C6, obtained by coupling strong sensitizing [Ir(coumarin 6)2(bpy)]+ with Ni−Sb9 POM with extremely exposed nickel site [NiO3(H2O)3], can drive H2 evolution with a turnover number of 326923, representing a record value among all the POM@MOF composite photocatalysts. This performance is over 34 times higher than that of the typical Ni4P2@UiO−Ir constructed from [Ir(ppy)2(bpy)]+ and Ni4P2 POM. Systematical investigations revealed that dual regulation of sensitizing and catalytic centers endowed Ni−Sb9@UiO−Ir−C6 with strong visible‐light absorption, efficient inter‐component electron transfer and high catalytic activity to concurrently promote H2 evolution. This work opens up a new avenue to develop highly active POM@MOF photocatalysts by dual regulation of sensitizing/catalytic centers at the molecular level.
Pressure‐Engineered Through‐Space Conjugation for Precise Control of Clusteroluminescence
Authors: Wang Yayun , Xiong Zuping , Wang Yanan , Li Aisen , Fang Yuanyuan , Li Lei , Wang Kai , Li Qian , Zhang Haoke
Published: November 2024

Clusteroluminogens (CLgens) represent an innovative class of nonconjugated luminophores that address the limitations of conventional π‐conjugated molecules. Different from the through‐bond conjugation mechanism in π‐conjugated luminophores, through‐space conjugation (TSC) plays dominant roles in CLgens. However, precisely controlling TSC to customize the optical properties of CLgens remains a significant challenge. This work proposes a novel strategy of high pressure to engineer TSC within tetraphenylalkanes (TPAs)‐based CLgens at molecular level. High‐pressure exploration enables accurate manipulation of clusteroluminescence and elucidates the intrinsic structure–property relationships involved. Upon initial compression, the predominant molecular distortions marked by increased interfacial angles between benzene rings diminish TSC, resulting in anomalous hypochromatic shift in emission. Subsequently, considerable structural contraction enhances TSC and suppresses molecular motion, resulting in a pronouncedly enhanced and bathochromic‐shifted emission. Notably, a series of TPAs‐based CLgens exhibit intense white‐light emission upon pressure release, attributed to irreversible structural distortion and destruction. This study not only advances the understanding of CLgens, but also underscores the crucial structural factors for effective TSC control, paving the way for establishing new photophysical theories for aggregate science.
Green Synthesis and Biological Study of Novel Cyclopenta[b]pyrrolizine: One‐Pot Multicomponent Reactions via Ag/Fe3O4@MWCNTs
Authors: Iravani Nasir
Published: November 2024

In this study, the cyclopenta[b]pyrrolizine was produced via using a nanocatalyst consisting of Ag/Fe3O4@MWCNTs in a multicomponent reaction that involved 2‐arylidenemalononitrile, ethyl 2‐amino‐4‐dioxo‐4‐arylbutanoates, alkyl bromides, and dimethyl acetylenedicarboxylate. The reaction was conducted in water at room temperature, resulting in the synthesis of new compounds. The synthesized compounds demonstrate antioxidant activity due to the occurrence of assessment procedures on its OH group. Moreover, an assessment was conducted on the antibacterial efficacy of recently synthesized pyridines using a disk diffusion method, employing two distinct strains of Gram‐negative bacteria. Notably, the tested compounds exhibited inhibitory effects on the growth of Gram‐positive bacteria as well.
Addressing a Labor and Delivery Unit Practice Gap Through a Count Sheet Revision
Authors: Caputo Amy L. , Faust Kristi
Published: November 2024

Unintentionally retained surgical items are never events that can be costly to patients and health care facilities. A labor and delivery unit quality improvement team at a southwestern Pennsylvania facility identified an opportunity for improvement associated with preventing retained surgical items. After reviewing the available literature, they identified a practice gap and decided to revise the count sheet. They standardized the existing sheet, shared it with frontline nurses for feedback and approval, and submitted it to leaders and the hospital's Forms Committee for approval. After an adequate quantity of the revised sheet was available for use, one member of the improvement team provided an educational session for nurses with practice time to use the revised count sheet. The team implemented the revised sheet and monitored compliance with its use. Compliance during and after the transition was 100%, and nurses provided positive feedback associated with using the revised sheet.
Caring for Patients With Pheochromocytomas in the Perioperative Setting
Authors: Criscitelli Theresa M.
Published: November 2024

Pheochromocytomas are rare, complex catecholamine‐secreting tumors of the adrenal medulla. Patients with pheochromocytomas may experience episodes of life‐threatening hypertension, and untreated tumors can be fatal. The nonspecific signs and symptoms (eg, headaches, palpitations, sweating) make diagnosing these tumors difficult. A comprehensive patient history, clinical evaluation during episodic hypertension, and biochemical test results can facilitate a definitive diagnosis. The only curative treatment is minimally invasive tumor removal. Because the tumor may recur, patients require follow‐up visits for approximately 10 years after surgery. Preoperative evaluations can include cardiac and imaging studies and genetic testing. Preoperative preparation involves controlling hypertension and planning for hypotension after tumor removal. Perioperative nurses should be prepared to assist anesthesia professionals with placing invasive hemodynamic monitors and responding to blood pressure changes. An interdisciplinary team can create a guideline or protocol for nurses to follow to enhance outcomes when caring for patients with pheochromocytomas.
Unveiling Electron‐Phonon and Electron‐Magnon Interactions in the Weak Itinerant Ferromagnet LaCo2P2
Authors: Usachov D. Yu. , Ali K. , Poelchen G. , Mende M. , Schulz S. , Peters M. , Bokai K. , Sklyadneva I. Yu. , Stolyarov V. , Chulkov E. V. , Kliemt K. , Paischer S. , Buczek P. A. , Heid R. , Hempel F. , Ruesing M. , Ernst A. , Krellner C. , Eremeev S. V. , Vyalikh D. V.
Published: November 2024

Studying and understanding many‐body interactions, particularly electron‐boson interactions, is essential for a deeper elucidation of fundamental physical phenomena and the development of novel material functionalities. Here, this aspect is explored in the weak itinerant ferromagnet LaCo2P2 by means of momentum‐resolved photoelectron spectroscopy (ARPES) and first‐principles calculations. The detailed ARPES patterns enable to unveil bulk and surface bands, spin splittings due to Rashba and exchange interactions, as well as the evolution of bands with temperature, which altogether creates a solid foundation for theoretical studies. The latter has allowed to establish the impact of electron‐boson interactions on the electronic structure, that are reflected in its strong renormalization driven by electron‐magnon interaction and the emergence of distinctive kinks of surface and bulk electron bands due to significant electron‐phonon coupling. Our results highlight the distinct impact of electron‐boson interactions on the electronic structure, particularly on the itinerant d states. Similar electronic states are observed in the isostructural iron pnictides, where electron‐boson interactions play a crucial role in the emergence of superconductivity. It is believed that further studies of material systems involving both magnetically active d‐ and f‐sublattices will reveal more advanced phenomena in the bulk and at distinct surfaces, driven by a combination of factors including Rashba and Kondo effects, exchange magnetism, and electron‐boson interactions.
A review of the non‐semiaquatic adaptations of extinct crocodylomorphs throughout their fossil record
Authors: Pochat‐Cottilloux Yohan
Published: November 2024

Crocodylomorphs constitute a clade of archosaurs that have thrived since the Mesozoic until today and have survived numerous major biological crises. Contrary to historic belief, their semiaquatic extant representatives (crocodylians) are not living fossils, and, during their evolutionary history, crocodylomorphs have evolved to live in a variety of environments. This review aims to summarize the non‐semiaquatic adaptations (i.e., either terrestrial or fully aquatic) of different groups from different periods, highlighting how exactly those different lifestyles are inferred for those animals, with regard to their geographic and temporal distribution and phylogenetic relationships. The ancestral condition for Crocodylomorpha seems to have been a terrestrial lifestyle, linked with several morphological adaptations such as an altirostral skull, long limbs allowing a fully erect posture and a specialized dentition for diets based on land. However, some members of this clade, such as thalattosuchians and dyrosaurids display adaptations for an opposite, aquatic lifestyle, interestingly inferred from the same type of morphological observations. Finally, new techniques for inferring the paleobiology of those extinct animals have been put forward in the last decade, appearing as a complementary approach to traditional morphological descriptions and comparisons. Such is the case of paleoneuroanatomical (CT scan data), histological, and geochemical studies.
Functional and phylogenetic signals in the pectoral girdle of Thalattosuchia and Dyrosauridae (Crocodylomorpha)
Authors: Scavezzoni Isaure , Johnson Michela M. , Jouve Stéphane , Fischer Valentin
Published: November 2024

Crocodylomorphs have colonized various environments from fully terrestrial to fully aquatic, making it an important clade among archosaurs. A remarkable example of the rich past diversity of Crocodylomorpha Hay, 1930 is the marine colonization undergone by several crocodylomorph lineages, particularly Thalattosuchia Fraas, 1901 during the Early Jurassic–Early Cretaceous, and Dyrosauridae de Stefano, 1903 during the Late Cretaceous–Early Eocene. Thalattosuchia represents the most impressive and singular marine radiation among Crocodylomorpha, occupying various ecological niches, before enigmatically disappearing in the Cretaceous. Dyrosauridae, on the other hand, is known for surviving the end‐Cretaceous mass extinction in abundance but subsequently vanished. The evolutionary path undertaken by crocodylomorphs into the aquatic environments and the reasons for their disappearance outside marine extinction events during the Mesozoic remains a mystery. Despite a well‐preserved fossil record, attention has primarily centered on craniodental adaptations, overlooking the swimming‐related adaptations recorded in the postcranial skeleton. This research primarily involves a comprehensive examination of the pectoral girdle of the most representative members of Thalattosuchia and Dyrosauridae, highlighting their evolutionary trajectories over time. Additionally, this work aims to test the phylogenetic signal residing in the postcranial anatomy of Crocodylomorpha. As such, the most recent and complete Crocodylomorpha phylogenetic dataset has been repurposed: 42 new postcranial characters have been added and several others have been revised to address our phylogenetic question. We stress that postcranial anatomy constitutes an important tool supply to better understand the relations of extinct crocodyliforms, but also offers insights on their development, ecology, and biomechanics.