bluuebunny/crossref_metadata_2025_split huggingface dataset:
Multifunctional Molecular Design of a New Fulleropyrrolidine Electron Transport Material Family Engenders High Performance of Perovskite Solar Cells
Authors: Xing Zhou , Liu Fu , Li Shu‐Hui , Chen Zuo‐Chang , An Ming‐Wei , Zheng Shizhao , Jen Alex K.‐Y. , Yang Shihe 
Published: September 2021

Abstract[6,6]‐phenyl‐C61‐butyric acid methyl ester remains indispensable as the electron transport material (ETM) for perovskite solar cells (PSCs), but its synthesis involves complicated multisteps with low productivity. In contrast, the potential of synthesizing simpler fulleropyrrolidine derivatives has long been overlooked, and little has been understood regarding their structure‐dependent effects on photovoltaic (PV) performance. Herein, seven novel fulleropyrrolidine derivatives (F1–F7) are deliberately designed, synthesized, and comprehensively characterized in both solution and thin‐film states and subsequently investigated as ETMs for PSCs. Notably, the F4 delivers the highest power conversion efficiencies over 20% of devices, which surpass all reported fulleropyrrolidine ETMs due to its optimal photoelectric property. Moreover, the structure‐dependent effects of the fullerenes on PV parameters are uncovered, including solubility, intermolecular interaction, packing structure, and charge‐transfer ability, which can guide the future design of high‐performance and stable fullerene ETMs for PSCs.
pH‐Sensitive Molecular‐Switch‐Containing Polymer Nanoparticle for Breast Cancer Therapy with Ferritinophagy‐Cascade Ferroptosis and Tumor Immune Activation
Authors: Zuo Tiantian , Fang Tianxu , Zhang Jun , Yang Jie , Xu Rui , Wang Zhihua , Deng Huizi , Shen Qi 
Published: September 2021

AbstractFerritin internalized into tumor cells is degraded and releases iron ions via ferritinophagy. Iron ions participate in Fenton reaction to produce reactive oxygen species for lipid peroxidation and ferroptosis. Inhibition of indoleamine‐2,3‐dioxygenase (IDO) decreases tryptophan elimination to induce T cells activation for tumor immunosuppression relief. The active tumor targeting nanoparticles containing ferritin and a pH‐sensitive molecular‐switch (FPBC@SN) are developed to utilize ferritinophagy‐cascade ferroptosis and tumor immunity activation for cancer therapy. FPBC@SN disintegrates in acidic cytoplasm and releases sorafenib (SRF) and IDO inhibitor (NLG919). SRF upregulates nuclear receptor coactivator 4 (NCOA4) to induce ferritin and endogenous iron pool degradation by ferritinophagy, then obtained iron ions participate in the Fenton reaction to produce lipid peroxide (LPO). Meanwhile, SRF blocks glutathione synthesis to downregulate glutathione peroxidase 4 (GPX4) which can scavenge LPO as a different pathway from ferritinophagy to promote ferroptosis in tumor cells. NLG919 inhibits IDO to reduce tryptophan metabolism, so immunity in tumors is aroused to anti‐tumor. In vitro and in vivo experiments prove FPBC@SN inhibits tumor cell growth and metastasis, indicating the potential of FPBC@SN for breast cancer therapy based on the combination of ferritinophagy‐cascade ferroptosis and tumor immunity activation.
Atomically Dispersed High‐Density Al–N4 Sites in Porous Carbon for Efficient Photodriven CO2 Cycloaddition
Authors: Yang Qihao , Peng Huaitao , Zhang Qiuju , Qian Xu , Chen Xu , Tang Xuan , Dai Sheng , Zhao Jiajun , Jiang Kun , Yang Qiu , Sun Jian , Zhang Linjuan , Zhang Nian , Gao Honglin , Lu Zhiyi , Chen Liang 
Published: September 2021

AbstractHighly active catalysts that can directly utilize renewable energy (e.g., solar energy) are desirable for CO2 value‐added processes. Herein, aiming at improving the efficiency of photodriven CO2 cycloaddition reactions, a catalyst composed of porous carbon nanosheets enriched with a high loading of atomically dispersed Al atoms (≈14.4 wt%, corresponding to an atomic percent of ≈7.3%) coordinated with N (AlN4 motif, Al–N–C catalyst) via a versatile molecule‐confined pyrolysis strategy is reported. The performance of the Al–N–C catalyst for catalytic CO2 cycloaddition under light irradiation (≈95% conversion, reaction rate = 3.52 mmol g−1 h−1) is significantly superior to that obtained under a thermal environment (≈57% conversion, reaction rate = 2.11 mmol g−1 h−1). Besides the efficient photothermal conversion induced by the carbon matrix, both experimental and theoretical analysis reveal that light irradiation favors the photogenerated electron transfer from the semiconductive Al–N–C catalyst to the epoxide reactant, facilitating the formation of a ring‐opened intermediate through the rate‐limiting step. This study not only provides an advanced Al–N–C catalyst for photodriven CO2 cycloaddition, but also furnishes new insight for the rational design of superior photocatalysts for diverse heterogeneous catalytic reactions in the future.
Monolayer Support Control and Precise Colloidal Nanocrystals Demonstrate Metal–Support Interactions in Heterogeneous Catalysts
Authors: Goodman Emmett D. , Asundi Arun S. , Hoffman Adam S. , Bustillo Karen C. , Stebbins Jonathan F. , Bare Simon R. , Bent Stacey F. , Cargnello Matteo 
Published: September 2021

AbstractElectronic and geometric interactions between active and support phases are critical in determining the activity of heterogeneous catalysts, but metal–support interactions are challenging to study. Here, it is demonstrated how the combination of the monolayer‐controlled formation using atomic layer deposition (ALD) and colloidal nanocrystal synthesis methods leads to catalysts with sub‐nanometer precision of active and support phases, thus allowing for the study of the metal–support interactions in detail. The use of this approach in developing a fundamental understanding of support effects in Pd‐catalyzed methane combustion is demonstrated. Uniform Pd nanocrystals are deposited onto Al2O3/SiO2 spherical supports prepared with control over morphology and Al2O3 layer thicknesses ranging from sub‐monolayer to a ≈4 nm thick uniform coating. Dramatic changes in catalytic activity depending on the coverage and structure of Al2O3 situated at the Pd/Al2O3 interface are observed, with even a single monolayer of alumina contributing an order of magnitude increase in reaction rate. By building the Pd/Al2O3 interface up layer‐by‐layer and using uniform Pd nanocrystals, this work demonstrates the importance of controlled and tunable materials in determining metal–support interactions and catalyst activity.
Polydopamine Nanobottles with Photothermal Capability for Controlled Release and Related Applications
Authors: Qiu Jichuan , Shi Yifeng , Xia Younan 
Published: September 2021

AbstractNanobottles refer to colloidal particles featuring a hollow body connected to a single opening on the surface. This unique feature makes them ideal carriers for the encapsulation and controlled release of various types of cargos. Here a facile route to the fabrication of uniform nanobottles made of polydopamine by leveraging swelling‐induced pressure is reported. When polystyrene spheres are coated with polydopamine and then incubated with a toluene/water emulsion, the polystyrene will be swollen to automatically poke a single hole in the shell because of the pressure inside the shell. After quenching the swelling with ethanol and then removing all the polystyrene with tetrahydrofuran, polydopamine nanobottles are obtained. The dimensions of the hollow body are determined by the polystyrene template, while the size of the opening can be tuned by varying the shell thickness. Through the opening, different types of cargos, including small molecules and biomacromolecules, can be easily loaded with a thermoresponsive material into the cavity. The cargos can be released in a controllable manner through direct heating or polydopamine‐enabled photothermal heating. In a proof‐of‐concept experiment, the polydopamine nanobottles are used for temperature‐controlled release of thrombin to trigger the formation of fibrin gels in situ.
Atomically Dispersed Ruthenium on Nickel Hydroxide Ultrathin Nanoribbons for Highly Efficient Hydrogen Evolution Reaction in Alkaline Media
Authors: Chen Xiaoyu , Wan Jiawei , Wang Jin , Zhang Qinghua , Gu Lin , Zheng Lirong , Wang Na , Yu Ranbo 
Published: September 2021

AbstractAchieving highly efficient hydrogen evolution reaction (HER) in alkaline media is a great challenge. Single‐atom catalysts with high‐loading amount have attracted great interest due to their remarkable catalytic properties. Herein, by using nickel foam as the substrate, the authors design and precisely synthesize atomic ruthenium (Ru)‐loaded nickel hydroxide ultrathin nanoribbons (R‐NiRu) with a high atomic Ru loading amount reaching ≈7.7 wt% via a one‐step hydrothermal method. The presence of concentrated Cl− in the synthetic system is beneficial for constructing ultrathin nanoribbons, which, with abundant edge OH groups, make it easy to trap atomic Ru. Taking advantage of the synergy between atomic Ru and the nanoribbon morphology of nickel hydroxide, R‐NiRu exhibit a low overpotential of 16 mV for HER at 10 mA cm−2 and a Tafel slope of 40 mV dec−1 in aqueous 1.0 m KOH solution, which are superior to those of commercial Pt/C (overpotential of 17 mV at 10 mA cm−2, Tafel slope of 43 mV dec−1). Density functional theory (DFT) calculation results demonstrate that atomically dispersed Ru can significantly reduce the HER energy barrier. Moreover, R‐NiRu maintains exceptional stability after 5000 cyclic voltammetry cycles. This efficient and facile synthetic strategy provides a new avenue for designing efficient catalysts.
Ultrathin Covalent Organic Framework Membranes via a Multi‐Interfacial Engineering Strategy for Gas Separation
Authors: Ying Yunpan , Peh Shing Bo , Yang Hao , Yang Ziqi , Zhao Dan 
Published: September 2021

AbstractCovalent organic frameworks (COFs) are promising membrane materials due to their high porosity, ordered arrangements, and high stability. However, the relatively large pore size and complicated membrane preparation processes of COFs limit their applications in sieving small gas molecules, even at a lab scale. Herein, a multi‐interfacial engineering strategy is proposed, that is, direct layer‐by‐layer interfacial reaction of two COFs (TpPa‐SO3H and TpTGCl) with different pore sizes to form narrowed apertures at the COF–COF interfaces atop a relatively large‐pore COF (COF‐LZU1) film. At 423 K, one fabricated 155 nm‐thick ultrathin COF membrane displays H2 permeance as high as 2163 gas permeation units (GPU) and a H2/CO2 selectivity of 26, transcending the 2008 Robeson upper bound. This strategy not only provides high‐performance membrane candidates for H2 separation, but also enlightens the interfacial engineering and pore engineering manipulation for other COFs, porous polymers, and their membranes.
High Energy Density Solid State Lithium Metal Batteries Enabled by Sub‐5 µm Solid Polymer Electrolytes
Authors: He Fei , Tang Wenjing , Zhang Xinyue , Deng Lijun , Luo Jiayan 
Published: September 2021

AbstractSolid‐state batteries (SSBs) are considered as the most promising next‐generation high‐energy‐density energy storage devices due to their ability in addressing the safety concerns from organic electrolytes and enabling energy dense lithium anodes. To ensure the high energy density of SSBs, solid‐state electrolytes (SSEs) are required to be thin and light‐weight, and simultaneously offer a wide electrochemical window to pair with high‐voltage cathodes. However, the decrease of SSE thickness and delicate structure may increase the cell safety risks, which is detrimental for the practical application of SSBs. Herein, to demonstrate a high‐energy‐density SSB with sufficient safety insurance, an ultrathin (4.2 µm) bilayer SSE with porous ceramic scaffold and double‐layer Li+‐conducting polymer, is proposed. The fire‐resistant and stiff ceramic scaffold improves the safety capability and mechanical strength of the composite SSE, and the bilayer polymer structure enhances the compatibility of Li metal anode and high‐voltage cathodes. The 3D ceramic facilitates Li‐ion conduction and regulates Li deposition. Thus, high energy density of 506 Wh kg−1 and 1514 Wh L−1 is achieved based on LiNi0.8Co0.1Mn0.1O2 (NCM811) cathodes with a low N/P ratio and long lifespan over 3000 h. High‐energy‐density anode‐free cells are further demonstrated.
Virus‐Mimic mRNA Vaccine for Cancer Treatment
Authors: Meng Chaoyang , Chen Zhe , Mai Junhua , Shi Qing , Tian Shaohui , Hinkle Louis , Li Jun , Zhang Zhe , Ramirez Maricela , Zhang Licheng , Xu Yitian , Zhang Jilu , Pan Ping‐Ying , Chen Shu‐Hsia , Li Hangwen , Shen Haifa 
Published: September 2021

AbstractAn effective therapeutic cancer vaccine should be empowered with the capacity to overcome the immunosuppressive tumor microenvironment. Here, the authors describe a mRNA virus‐mimicking vaccine platform that is comprised of a phospholipid bilayer encapsulated with a protein‐nucleotide core consisting of antigen‐encoding mRNA molecules, unmethylated CpG oligonucleotides and positively charged proteins. In cell culture, VLVP potently stimulated bone marrow‐derived dendritic cells (BMDCs) to express inflammatory cytokines that facilitated dendritic cell (DC) maturation and promoted antigen processing and presentation. In tumor‐bearing mice, VLVP treatment stimulated proliferation of antigen‐specific CD8+T cells in the lymphatic organs and T cell infiltration into the tumor bed, resulting in potent anti‐tumor immunity. Cytometry by time of flight (CyTOF) analysis revealed that VLVP treatment stimulated a 5‐fold increase in tumor‐associated CD8+DCs and a 4‐fold increase in tumorinfiltrated CD8+T cells, with concurrent decreases in tumor‐associated bone marrow‐derived suppressor cells and arginase 1‐ expressing suppressive DCs. Finally, CpG oligonucleotide is an essential adjuvant for vaccine activity. Inclusion of CpG not only maximized vaccine activity but also prevented PD‐1 expression in T cells, serving the dual roles as a potent adjuvant and a checkpoint blockade agent.
2021 Update on allogeneic hematopoietic stem cell transplant for myelofibrosis: A review of current data and applications on risk stratification and management
Authors: Ali Haris , Bacigalupo Andrea 
Published: September 2021

AbstractThe number of patients with myelofibrosis (MF) undergoing an allogeneic hemopoietic stem cell transplantation (HSCT) is increasing: in the analysis of the European Group for Blood and Marrow Transplantation (EBMT) the number of MF has increased from 515 in 2014 to 748 in 2018 . This reflects the fact that HSCT is currently the only curative treatment, capable of inducing prolonged disease‐free survival. Nevertheless, several problems prevent more patients from undergoing an allogeneic HSCT: we will be discussing indications for HSCT, comorbidities, splenomegaly, older age and disease phase. Donor type and stem cell source are less of a problem. Several transplant platforms exist, including different strategies for graft versus host disease (GvHD) prophylaxis, Age tailored conditioning regimens need to be implemented, to allow older and fragile patients to undergo an allogeneic HSCT.
Impact of the coronavirus pandemic on mental health and health care in adults with neurofibromatosis: Patient perspectives from an online survey
Authors: Wolters Pamela L. , Reda Stephanie , Martin Staci , Al Ghriwati Nour , Baker Melissa , Berg Dale , Erickson Gregg , Franklin Barbara , Merker Vanessa L. , Oberlander Beverly , Reeve Stephanie , Rohl Claas , Rosser Tena , Toledo‐Tamula Mary Anne , Vranceanu Ana‐Maria 
Published: September 2021

AbstractThe coronavirus pandemic increased anxiety and stress and prevented access to health care worldwide; it is unclear how COVID‐19 affected adults with a multisystem genetic disorder such as neurofibromatosis (NF). An anonymous online survey was distributed through an international registry and foundations to adults with NF (June–August 2020) to assess the impact of the pandemic on mental health and NF health care. Six hundred and thirteen adults (18–81 years; M = 45.7) with NF1 (77.8%), NF2 (14.2%), and schwannomatosis (7.8%) provided complete responses. Respondents rated moderate‐to‐high amounts of worry about the impact of COVID‐19 on their emotional (46.3%) and physical health (46.7%), and 54.8% endorsed moderate‐to‐high pandemic‐related stress. Adults with diagnosed/suspected mental health disorders or moderate‐to‐severe NF symptom impact as well as females endorsed higher COVID‐19 stress (ps < 0.01). Less than half who missed a doctor's appointment for their NF care (43.4%) used telehealth. Of these, 33.3% and 46.2% reported that telehealth met their needs to a moderate or high degree, respectively. Results indicated that subgroups of adults with NF experience higher COVID‐19‐related worries and stress and may need additional support. Furthermore, telehealth is under‐utilized and could help NF providers connect with patients, although improved delivery and patient training may facilitate expanded use of these services.
4′‐Selenonucleosides: Regio‐ and Stereoselective Synthesis of Novel Ribavirin and Acadesine Analogs as Anti‐Hepatitis C Virus (HCV) Agents
Authors: Lee Hyejin , Jarhad Dnyandev B. , Lee Ahrim , Lee Choongho , Jeong Lak Shin 
Published: September 2021

AbstractIntrigued by the biological activity of 2′‐C‐methylribofuranosyl nucleosides, and ribavirin/acadesine, based on the bioisosteric rationale between oxygen and selenium, we herein report a design and synthesis of the 2′‐C‐methyl‐4′‐seleno‐ribavirin and ‐acadesine as potential anti‐HCV agents. The 2′‐C‐methyl 4′‐selenoribavirin was synthesized in a regio‐ and stereoselective manner and completely characterized through 2D NMR and X‐ray crystallography. While the 2′‐C‐methyl 4′‐selenoacadesine has been efficiently synthesized by utilizing purine‐ring opening/degradation procedure via nucleophilic cleavage of N3−C2 bond of a purine by ethylenediamine (EDA) as the key step.
Advanced do‐not‐attempt‐resuscitation directives and emergency medical services for out‐of‐hospital cardiopulmonary arrest patients in Japan: a pilot study
Authors: Maruhashi Takaaki , Oi Marina , Asakuma Sadataka , Kotoh Rika , Shibuya Hirotaka , Kurihara Yutaro , Asari Yasushi 
Published: September 2021

AimsWe investigated how do‐not‐attempt‐resuscitation (DNAR) orders are currently used, and we examined the emergency medical team responses for out‐of‐hospital cardiac arrest (OHCA) cases in Japan.MethodsThe sample for this prospective study comprised all OHCA cases attended to by the Sagamihara Municipal Fire Department emergency medical services between May 30, 2019 and February 15, 2020. Data were recorded by the responding emergency medical team.ResultsThere were 396 OHCA cases. The mean age was 75 ± 18 years, and individuals aged 65 years or older accounted for 80.6%. Approximately 70% of the patients had an underlying disease. A DNAR order was available in only 45 (11.4%) of the cases, of which 12 (26.7%) were written, 27 (60%) were verbally confirmed, and six (13.3%) were confirmed in some other way or both. The home physician was present and able to confirm the patient’s death in only one of the DNAR cases. In 43 (95.6%) of the cases, the emergency medical team carried out cardiopulmonary resuscitation despite a DNAR order; of them, a total of 17 (37.8%) patients were transported to a tertiary emergency hospital.ConclusionsOur analyses indicate the under‐utilization of DNAR advance directives and advance care planning (which are important for better end‐of‐life care) in Japan. Currently, an emergency medical team could be required to attempt resuscitation against an individuals’ clear DNAR order. In the future, legal arrangements regarding the handling of DNAR directives on site may be required to respect patients’ wishes.
Plasmon‐Enhanced, Self‐Traced Nanomotors on the Surface of Silicon
Authors: Yang Jianhua , Zheng Jiapeng , Ai Ruoqi , Lai Yunhe , Chow Tsz Him , Shao Lei , Wang Jianfang 
Published: September 2021

AbstractLight‐driven nanomotors have attracted much attention due to their potential applications. The movement of conventional nanomotors typically occurs in the solution phase, which limits their application fields. Utilizing visible light to drive nanomotors at the solid–liquid interface represents a grand challenge due to the large friction force between the nanomotor and the solid surface. Based on the attractive plasmon resonance of Au nanocrystals, for the first time, plasmon‐enhanced Au nanocrystal‐based nanomotors moving at the silicon–aqueous solution interface have been developed. Such nanomotors move with a clear trace engraved on the Si surface, representing an excellent and exceptional self‐traced nanomotor system. In addition, the nanomotor trace on the Si surface also provides a unique and promising approach to the fabrication of nanoscale Si patterns, which is central to many applications, including microelectronics, sensing, information storage, and optoelectronics.
Tuning and Directing Energy Transfer in the Whole Visible Spectrum through Linker Installation in Metal–Organic Frameworks
Authors: Ren Daming , Xia Hai‐Lun , Zhou Kang , Wu Shenjie , Liu Xiao‐Yuan , Wang Xiaotai , Li Jing 
Published: September 2021

AbstractWhile limited choice of emissive organic linkers with systematic emission tunability presents a great challenge to investigate energy transfer (ET) over the whole visible light range with designable directions, luminescent metal‐organic frameworks (LMOFs) may serve as an ideal platform for such study due to their tunable structure and composition. Herein, five Zr6 cluster‐based LMOFs, HIAM‐400X (X=0, 1, 2, 3, 4) are prepared using 2,1,3‐benzothiadiazole and its derivative‐based tetratopic carboxylic acids as organic linkers. The accessible unsaturated metal sites confer HIAM‐400X as a pristine scaffold for linker installation. Six full‐color emissive 2,1,3‐benzothiadiazole and its derivative‐based dicarboxylic acids (L) were successfully installed into HIAM‐400X matrix to form HIAM‐400X‐L, in which the ET can be facilely tuned by controlling its direction, either from the inserted linkers to pristine MOFs or from the pristine MOFs to inserted linkers, and over the whole range of visible light. The combination of the pristine MOFs and the second linkers via linker installation creates a powerful two‐dimensional space in tuning the emission via ET in LMOFs.
Site‐Fixed Hydroboration of Terminal and Internal Alkenes using BX3/iPr2NEt**
Authors: Li Sida , Hu Chenyang , Cui Xin , Zhang Jiong , Liu Liu Leo , Wu Lipeng 
Published: September 2021

AbstractAn unprecedented and general hydroboration of alkenes with BX3 (X=Br, Cl) as the boration reagent in the presence of iPr2NEt is reported. The addition of iPr2NEt not only suppresses alkene polymerization and haloboration side reactions but also provides an “H” source for hydroboration. More importantly, the site‐fixed installation of a boryl group at the original position of the internal double bond is readily achieved in contrast to conventional transition‐metal‐catalyzed hydroboration processes. Further application to the synthesis of 1,n‐diborylalkanes (n=3–10) is also demonstrated. Preliminary mechanistic studies reveal a major reaction pathway that involves radical species and operates through a frustrated Lewis pair type single‐electron‐transfer mechanism.