bluuebunny/crossref_metadata_2025_split huggingface dataset:
Mesoporous PdN Alloy Nanocubes for Efficient Electrochemical Nitrate Reduction to Ammonia
Authors: Sun Lizhi , Liu Ben 
Published: October 2022

AbstractDeveloping highly active and selective electrocatalysts for electrochemical nitrate reduction reaction (NITRR) is very important for synthesizing recyclable ammonia (NH3) in an economic and environmentally friendly manner. Despite some encouraging progress, their activity and selectivity have been remarkably slower than expected. In this manuscript, mesoporous palladium‐nonmetal (meso‐PdX) nanocubes (NCs) are reported as a new series of highly efficient electrocatalysts for selective nitrate reduction reaction (NITRR) electrocatalysis to NH3. The samples feature uniformly alloyed compositions and highly penetrated mesopores with abundant highly active sites and optimized electronic structures. The best meso‐PdN NCs hold an outstanding NITRR activity and selectivity with a remarkable NH3 Faradaic efficiency of 96.1% and a yield rate of 3760 µg h−1 mg−1, suppressing the state‐of‐the‐art electrocatalysts. Meanwhile, meso‐PdN NCs are electrocatalytically stable, retaining well the activity and selectivity of NO3−‐to‐NH3 electrocatalysis for more than 20 cycles. Detailed mechanism studies ascribe the superior performance to combined compositional and structural synergies of meso‐PdN NCs that not only promote the adsorption (reactivity) of NO3− and the desorption of NH3 but also increase the retention time of key intermediates for the deeper NITRR electrocatalysis to NH3 through an eight‐electron pathway.
Dynamic Sustainable Polyimide Film Combining Hardness with Softness via a “Mimosa‐Like” Bionic Strategy
Authors: Wan Baoquan , Yang Xing , Dong Xiaodi , Zheng Ming‐Sheng , Zhao Quanliang , Zhang Hongkuan , Chen George , Zha Jun‐Wei 
Published: October 2022

AbstractDielectric polyimides (PIs) are ubiquitous as insulation in electrical power systems and electronic devices. Generally, dynamic polyimide is required to solve irreversible failure processes of electrical or mechanical damage, for example, under high temperature, pressure, and field strength. The challenge lies in the design of the molecular structure of rigid polyimide to achieve dynamic reversibility. Herein, a low‐molecular‐weight polyimide gene unit is designed to crosslink with polyimide ligase to prepare the smart film. Interestingly, due to the variability of gene unit and ligase combinations, the polyimide films combining hardness with softness are designed into three forms via a “Mimosa‐like” bionic strategy to adapt to different application scenarios. Meanwhile, the films have good degradation efficiency, excellent recyclability, and can be self‐healable, which makes them reuse. Clearly, the films can be used in the preparation of ultrafast sensors with a response time ≈0.15 s and the application of corona‐resistant films with 100% recovery. Furthermore, the construction of polyimide and carbon‐fiber‐reinforced composites (CFRCs) has been verified to apply to the worse environment. Nicely, the composites have the property of multiple cycles and the non‐destructive recycle rate of carbon fiber (CF) is as high as 100%. The design idea of preparing high‐strength dynamic polyimide by crosslinking simple polyimide gene unit with ligase could provide a good foundation and a clear case for the sustainable development of electrical and electronic polyimides, from the perspective of Mimosa bionics.
Controlled Fabrication of Carbon Nanotube Microspheres from Emulsion Templates: Exploring the Dynamics of Solvent Loss and Nanoparticle Assembly
Authors: Sanders Kate A. , De Volder Michael F. L. 
Published: October 2022

AbstractThe use of emulsions as templates for nanomaterial assembly is a versatile method to create controlled microstructures. However, production rates are often low, particularly where the droplet phase solvent must be removed to achieve consolidation. Here, the emulsion templated fabrication of microparticles from multi‐walled carbon nanotubes (CNTs) is studied. As an exemplar primary nanoparticle for microparticle assembly, CNTs present particular challenges due to their strong inter‐particle interactions and limited dispersion in solvents. Nevertheless, small batches of CNT microparticles have demonstrated promising performances in energy storage, environmental remediation, and sensing due to their controlled structures. Improving CNT microparticle production through emulsion processing is therefore interesting to promote these real‐world applications. In this work, it is shown that the slow rate of CNT microparticle formation from water‐in‐oil emulsions is due to spontaneous emulsification. Then methanol‐in‐oil emulsions are tested, which rapidly form fragile CNT capsules. Using mixtures of methanol and water, a faster rate of solvent loss can be balanced alongside nanoparticle assembly; CNT microparticle formation is up to twice as fast using 40% methanol compared to aqueous dispersions. In addition to facilitating faster CNT microparticle production, these findings offer more broadly applicable insights into the mechanisms of solvent transport in emulsions.
Soft Underwater Swimming Robots Based on Artificial Muscle
Authors: Wang Ruiqian , Zhang Chuang , Zhang Yiwei , Tan Wenjun , Chen Wenyuan , Liu Lianqing 
Published: October 2022

AbstractWith the increasing requirements of underwater missions and the rapid development of soft robotics technologies, soft underwater swimming robots have become a hot topic of research due to their low noise, high flexibility, and high environmental adaptability. In the past 10 years, research into soft underwater robots based on artificial muscle actuation has made considerable progress. Herein, a comprehensive survey on recent advances in soft underwater swimming robots based on different actuation methods is reviewed systematically, including pressure actuation, intelligent material actuation, and biomaterial actuation. First, for each type of actuation, the actuating principle, structural design, and swimming performance of soft underwater robots are introduced in detail. Then, according to the different swimming modes of underwater organisms, the aforementioned soft underwater robots are classified and compared. The results show that for different swimming tasks and application scenarios, the robot needs to realize the optimal design by reasonably selecting the actuating method and the swimming mode. This review summarizes the advanced information and critical technology in designing high‐performance soft underwater robots in the aspect of structural design, actuating methods, and swimming modes and offers an insightful outlook for the future development of soft robots.
Toward a Deeper Understanding of Gut Microbiome in Depression: The Promise of Clinical Applicability
Authors: Liu Lanxiang , Wang Haiyang , Zhang Hanping , Chen Xueyi , Zhang Yangdong , Wu Ji , Zhao Libo , Wang Dongfang , Pu Juncai , Ji Ping , Xie Peng 
Published: October 2022

AbstractThe emergence of the coronavirus disease 2019 pandemic has dramatically increased the global prevalence of depression. Unfortunately, antidepressant drugs benefit only a small minority of patients. Thus, there is an urgent need to develop new interventions. Accumulating evidence supports a causal relationship between gut microbiota dysbiosis and depression. To advance microbiota‐based diagnostics and therapeutics of depression, a comprehensive overview of microbial alterations in depression is presented to identify effector microbial biomarkers. This procedure generated 215 bacterial taxa from humans and 312 from animal models. Compared to controls, depression shows significant differences in β‐diversity, but no changes in microbial richness and diversity. Additionally, species‐specific microbial changes are identified like increased Eggerthella in humans and decreased Acetatifactor in rodent models. Moreover, a disrupted microbiome balance and functional changes, characterized by an enrichment of pro‐inflammatory bacteria (e.g., Desulfovibrio and Escherichia/Shigella) and depletion of anti‐inflammatory butyrate‐producing bacteria (e.g., Bifidobacterium and Faecalibacterium) are consistently shared across species. Confounding effects of geographical region, depression type, and intestinal segments are also investigated. Ultimately, a total of 178 species and subspecies probiotics are identified to alleviate the depressive phenotypes. Current findings provide a foundation for developing microbiota‐based diagnostics and therapeutics and advancing microbiota‐oriented precision medicine for depression.
Charge generation in organic solar cells: Journey toward 20% power conversion efficiency
Authors: Tamai Yasunari 
Published: October 2022

AbstractThe power conversion efficiencies of organic solar cells (OSCs) have routinely lagged far behind those of their inorganic counterparts. However, owing to the enormous contributions of many researchers, the power conversion efficiencies of OSCs have rapidly improved and now exceed 19%. The charge generation mechanisms in OSCs have been heavily debated during this period while acquiring valuable knowledge. This review highlights fundamental and cutting‐edge research that rationalizes why OSCs can generate photocurrent so efficiently. In particular, a photophysicist's views on exciton diffusion to donor:acceptor interfaces, charge transfer at the donor:acceptor interface, and long‐range spatial dissociation of charge transfer states are discussed. Although a general consensus in this area has not been reached yet, recent time‐resolved spectroscopic measurements provide important photophysical insights that can help achieving a better understanding of the charge generation mechanism in OSCs. Based on these observations, future research directions for realizing further improvements in OSC performance are discussed.
Multi‐rate observer design and optimal control to maximize productivity of an industry‐scale fermentation process
Authors: Shah Parth , Sheriff M. Ziyan , Bangi Mohammed Saad Faizan , Kravaris Costas , Kwon Joseph Sang‐Il , Botre Chiranjivi , Hirota Junichi 
Published: October 2022

AbstractChemical industries focus primarily on profitable operations, resulting in growing attention and advances in the field of digital twins and optimal control algorithms. However, most industries still struggle due to a lack of physical sensors, infrequent measurements, and asynchronous sampling. Thus, in this work, we have designed a multi‐rate state observer for state estimation from plant measurements and developed a model predictive controller (MPC) that maximized the profitability of an industry‐scale fermentation process (fermenter volume < 378,500 L). Additionally, as the fermentation process is complex due to the use of microorganisms, which cannot be accurately captured using a first‐principles model, we utilize a previously developed hybrid model in the proposed MPC formulation. The MPC uses a GAMS‐MATLAB framework to determine the optimal input profiles while considering practical process constraints. It is shown using multiple datasets, that the MPC can increase productivity while also decreasing the plant operating cost.
Methodological correlates of variability in the prevalence of posttraumatic stress disorder in high‐risk occupational groups: A systematic review and meta‐regression
Authors: White Nicole , Wagner Shannon L. , Corneil Wayne , Fraess‐Phillips Alex , Krutop Elyssa , Fyfe Trina , Matthews Lynda R. , Randall Christine , Regehr Cheryl , White Marc , Alden Lynn E. , Buys Nicholas , Carey Mary G. 
Published: October 2022

AbstractBackgroundAlthough numerous studies have reported on PTSD prevalence in high‐risk occupational samples, previous meta‐analytic work has been severely limited by the extreme variability in prevalence outcomes.MethodsThe present systematic review and meta‐regression examined methodological sources of variability in PTSD outcomes across the literature on high‐risk personnel with a specific focus on measurement tool selection.ResultsThe pooled global prevalence of PTSD in high‐risk personnel was 12.1% [6.5%, 23.5%], and was similar to estimates obtained in other meta‐analytic work. However, meta‐regression revealed that PTSD prevalence differed significantly as a function of measurement tool selection, study inclusion criteria related to previous traumatic exposure, sample size, and study quality. PTSD prevalence estimates also differed significantly by occupational group and over time, as has also been reported in previous work, though exploratory examination of trends in measurement selection across these factors suggests that measurement strategy may partially explain some of these previously reported differences.ConclusionsOur results highlight a pressing need to better understand the role of measurement strategies and other methodological choices in characterizing variable prevalence outcomes. Understanding the role of methodological variance will be critical for work attempting to reliably characterize prevalence as well as risk and protective factors for PTSD.
Regioselective, Greener Protocol for the Synthesis of N‐Heterocyclic Compounds Catalyzed by Recyclable CuO NPs Coated with Ionic Liquid (CuO[HN222][Al2Cl7]
Authors: Kumar Parveen , Tomar Vijesh , Joshi Raj Kumar , Nemiwal Meena 
Published: October 2022

AbstractThe identification of purine‐derived ligands for a diversity of nucleotide‐dependent enzymes has assisted in enlightenment in interest in the synthesis of purine derivatives in recent decades. The research work discloses the synthesis of CuO NPs coated with ionic liquid (triethylammonium chloride (HN222) & aluminium chloride) as a novel and powerful nanocatalyst (CuO[HN222][Al2Cl7]) as well as the exploration of its activity in the synthesis of N‐arylnucleobase and N‐aryl heterocyclic derivatives by C−N cross‐coupling reaction between adenine, imidazole, and benzimidazole compounds with aryl boronic acids in greener solvent at room temperature. This practical approach produced the products with good to excellent yields in acceptable reaction time (3 h). The nanocatalyst was characterized by Brunauer‐Emmett‐Teller (BET), Energy‐dispersive X‐ray spectroscopy (EDS), Fourier‐transform infrared spectroscopy (FTIR), Scanning electron microscopy (SEM), Powder X‐ray diffraction (P‐XRD), and X‐ray photoelectron spectroscopy (XPS). Additional eco‐friendly aspects of this nanocatalyst include strong catalytic activity, ease of recovery of nanocatalyst from the reaction mixture via filtration, and recyclability upto five times without significant performance loss.
Two‐Dimensional Excitonic Networks Directed by DNA Templates as an Efficient Model Light‐Harvesting and Energy Transfer System
Authors: Zhou Xu , Satyabola Deeksha , Liu Hao , Jiang Shuoxing , Qi Xiaodong , Yu Lu , Lin Su , Liu Yan , Woodbury Neal W. , Yan Hao 
Published: October 2022

AbstractPhotosynthetic organisms organize discrete light‐harvesting complexes into large‐scale networks to facilitate efficient light collection and utilization. Inspired by nature, herein, synthetic DNA templates were used to direct the formation of dye aggregates with a cyanine dye, K21, into discrete branched photonic complexes, and two‐dimensional (2D) excitonic networks. The DNA templates ranged from four‐arm DNA tiles, ≈10 nm in each arm, to 2D wireframe DNA origami nanostructures with different geometries and varying dimensions up to 100×100 nm. These DNA‐templated dye aggregates presented strongly coupled spectral features and delocalized exciton characteristics, enabling efficient photon collection and energy transfer. Compared to the discrete branched photonic systems templated on individual DNA tiles, the interconnected excitonic networks showed approximately a 2‐fold increase in energy transfer efficiency. This bottom‐up assembly strategy paves the way to create 2D excitonic systems with complex geometries and engineered energy pathways.
CAPturAM, eine chemo‐enzymatische Strategie zur selektiven Detektion von physiologischen CAPAM‐Targets
Authors: Muthmann Nils , Albers Marvin , Rentmeister Andrea 
Published: October 2022

AbstractModifizierte Nukleotide beeinflussen eukaryontische mRNAs in allen Bereichen ihres Lebenszyklus und tragen zur Regulierung der Genexpression auf Transkriptions‐ und Translationsebene bei. An der 5′‐Kappe kommt Adenosin als erstes transkribiertes Nukleotid häufig als N6‐Methyl‐2′‐O‐methyladenosin (m6Am) vor. Dieser Modifikationstyp tritt gewebespezifisch und reversibel auf, was auf eine regulatorische Funktion hindeutet. CAPAM wurde als Methyltransferase identifiziert, die für die Bildung von m6Am verantwortlich ist, doch erweist sich die direkte Identifizierung ihrer Zieltranskripte als schwierig, da Antikörper nicht zwischen internem N6‐Methyladenosin (m6A) und m6Am unterscheiden können. Hier stellen wir CAPturAM vor, einen antikörperfreien chemisch‐biologischen Ansatz zur direkten Anreicherung und Detektion physiologischer CAPAM‐Targets. Wir nutzen die Promiskuität von CAPAM aus, um Propargylgruppen gezielt an seine Targets zu transferieren. Die anschließende Funktionalisierung ermöglicht die Anreicherung dieser Target‐RNAs. Unter Verwendung von Wildtyp‐ und CAPAM−/−‐Zellen wurde CAPturAM erfolgreich eingesetzt, um CAPAM‐Targets zu bestätigen oder zu widerlegen, was die gegenwärtige Überprüfung und Identifizierung von CAPAM‐Targets erleichtert.
The Single‐Component Flavin Reductase/Flavin‐Dependent Halogenase AetF is a Versatile Catalyst for Selective Bromination and Iodination of Arenes and Olefins**
Authors: Jiang Yuhua , Snodgrass Harrison M. , Zubi Yasmine S. , Roof Caitlin V. , Guan Yanfei , Mondal Dibyendu , Honeycutt Nicholas H. , Lee Johnny W. , Lewis Russell D. , Martinez Carlos A. , Lewis Jared C. 
Published: October 2022

AbstractFlavin‐dependent halogenases (FDHs) natively catalyze selective halogenation of electron rich aromatic and enolate groups. Nearly all FDHs reported to date require a separate flavin reductase to supply them with FADH2, which complicates biocatalysis applications. In this study, we establish that the single component flavin reductase/flavin dependent halogenase AetF catalyzes halogenation of a diverse set of substrates using a commercially available glucose dehydrogenase to drive its halogenase activity. High site selectivity, activity on relatively unactivated substrates, and high enantioselectivity for atroposelective bromination and bromolactonization was demonstrated. Site‐selective iodination and enantioselective cycloiodoetherification was also possible using AetF. The substrate and reaction scope of AetF suggest that it has the potential to greatly improve the utility of biocatalytic halogenation.
Thiazole Imide‐Based All‐Acceptor Homopolymer with Branched Ethylene Glycol Side Chains for Organic Thermoelectrics
Authors: Shi Yongqiang , Li Jianfeng , Sun Hengda , Li Yongchun , Wang Yimei , Wu Ziang , Jeong Sang Young , Woo Han Young , Fabiano Simone , Guo Xugang 
Published: October 2022

Abstractn‐Type semiconducting polymers with high thermoelectric performance remain challenging due to the scarcity of molecular design strategy, limiting their applications in organic thermoelectric (OTE) devices. Herein, we provide a new approach to enhance the OTE performance of n‐doped polymers by introducing acceptor‐acceptor (A‐A) type backbone bearing branched ethylene glycol (EG) side chains. When doped with 4‐(2,3‐dihydro‐1,3‐dimethyl‐1H‐benzimidazol‐2‐yl)‐N,N‐dimethylbenzenamine (N‐DMBI), the A‐A homopolymer PDTzTI‐TEG exhibits n‐type electrical conductivity (σ) up to 34 S cm−1and power factor value of 15.7 μW m−1 K−2. The OTE performance of PDTzTI‐TEG is far greater than that of homopolymer PBTI‐TEG (σ=0.27 S cm−1), indicating that introducing electron‐deficient thiazole units in the backbone further improves the n‐doping efficiency. These results demonstrate that developing A‐A type polymers with EG side chains is an effective strategy to enhance n‐type OTE performance.
A Photoresponsive Battery Based on a Redox‐Coupled Covalent‐Organic‐Framework Hybrid Photoelectrochemical Cathode
Authors: Wang Wei , Zhang Xiang , Lin Jing , Zhu Lei , Zhou Enbo , Feng Yangyang , Yuan Daqiang , Wang Yaobing 
Published: October 2022

AbstractPhotoresponsive batteries promise flexible and low‐cost solar‐to‐electrochemical energy storage (SES), but suffer from a limited SES efficiency due to rapid charge recombination and sluggish redox. Here, we present a porous‐shell/core hybrid of covalent organic framework@carbon nanotube. This hybrid ensures long‐lived separated charges (τave=3.0 ns) by an electron transfer relay starting from the donor‐acceptor molecules to the nanoscale heterojunction. These charges are further allowed to drive high‐rate redox of −C=O/−C−O− and −C−N/−C=N+ with facile kinetics. Equipped with this photoelectrochemical cathode, a photoresponsive aqueous battery shows a 5‐fold enhancement in SES efficiency (1.1 % at 1 sun) over their counterparts. It is unveiled that the electron relay favors the formation of electron‐enriching −C−O− and hole‐enriching −C=N+ groups responsible for photoelectrochemical Zn2+ and OTf− storage cascade; and further, the general photo coupled ions transfer (PCIT) process is proposed. This work presents an inspiring photoelectrochemical cathode design and theoretical insight for photoresponsive batteries.
Stimuli‐Responsive RNA‐Cleaving DNAzyme for Biomedical Application
Authors: Wang Siyuan , Liu Yaqi , Shang Jinhua , Wang Huimin , Yang Changying , Liu Xiaoqing , Wang Fuan 
Published: October 2022

AbstractDNAzymes are synthetic deoxynucleotide oligomers with catalytic properties selected through in vitro systematic evolution of ligands by exponential enrichment (SELEX) technique. RNA‐cleaving DNAzymes have attracted increasing attentions in bioanalysis and biomedical applications due to their simple synthesis and modification, stable structure, and high catalytic activity. Especially, their different modes of activity regulation enable their extensive theranostic development. This review introduces the in vitro selection of DNAzymes and some typical ones, followed by the description of various stimuli‐responsive regulation strategies on DNAzyme activity, including metal ion cofactors, small molecules, protease, light, and heat. Then the recent advances of DNAzyme‐based biosensors, therapeutic applications, cell‐cell interaction regulation, and logic operation are summarized. At last, the current challenges and possible development of DNAzyme‐based biosensors are discussed.
V2O5 as a versatile electrode material for postlithium energy storage systems
Authors: Fu Qiang , Zhao Hainan , Sarapulova Angelina , Dsoke Sonia 
Published: October 2022

AbstractPostlithium batteries have received intense attention as an alternative for large‐scale electric energy storage systems due to their rich resources and low cost. Vanadium pentoxide (V2O5) is very promising as a host material because of its rich structure, high capacity, easy preparation, and adequate safety. V2O5 has several modifications, including α‐, β‐, δ‐, γ‐, ζ‐, and ε‐V2O5, as well as hydrate V2O5 (V2O5·nH2O). In this mini‐review, we comprehensively summarize the crystal structure of polymorphs V2O5 materials, their relationships, and their applications in postlithium batteries, including monovalent (Na+, K+), multivalent‐ion (Mg2+, Ca2+, Zn2+, Al3+), and nonmetallic (H+, NH4+)‐based batteries. Finally, general strategies are reviewed to improve the performance of V2O5.