bluuebunny/crossref_metadata_2025_split huggingface dataset:
Balance Effect: A Universal Strategy for Transition Metal Carbides to Enhance Hydrogen Evolution
Authors: Yang Chenfan , Shen Ke , Zhao Rong , Xiang Hui , Wu Jing , Zhong Wenda , Zhang Qin , Li Xuanke , Yang Nianjun 
Published: October 2021

AbstractHydrogen production from water splitting is one of the most promising approaches to achieve carbon neutrality when high‐performance electrocatalysts are ready for the sluggish hydrogen evolution reaction (HER). Although earth‐rich and cheap transition metal carbides (TMCs) are potential HER electrocatalysts, their platinum‐like electronic structures are severely hampered by their strong binding with hydrogen intermediates (H*). Here, a universal “balance effect” strategy is proposed, where nitrogen‐doped graphene (NG) is introduced to weaken the interactions of TMCs (M = Mo, W, Ti, and V) with H*. Hydrogen binding energies calculated by the density functional theory show that the TMCs coupled with NG appear to be thermo‐neutral. Stemming from different work functions of TMCs and NG, partial electrons transfer from TMC to the NG surface, resulting in optimized electronic structures of these electrocatalysts. These optimized electronic structures balance hydrogen adsorption and desorption, leading to synergistically‐enhanced HER kinetics. The overpotentials and Tafel slopes of the HER on these TMC@NG electrocatalysts are thus pronouncedly reduced in both acidic and alkaline solutions. This universal strategy provides a novel approach to design effective and stable TMCs as superior HER electrocatalysts. It can be expanded to other electrocatalysts for sustainable hydrogen production in different media.
Importance of High‐Electron Mobility in Polymer Acceptors for Efficient All‐Polymer Solar Cells: Combined Engineering of Backbone Building Unit and Regioregularity
Authors: Seo Soodeok , Sun Cheng , Lee Jin‐Woo , Lee Seungjin , Lee Dongchan , Wang Cheng , Phan Tan Ngoc‐Lan , Kim Geon‐U , Cho Shinuk , Kim Yun‐Hi , Kim Bumjoon J. 
Published: October 2021

AbstractThe charge transport ability of polymer acceptors (PAs) is crucial for achieving high power conversion efficiencies (PCEs) of all‐polymer solar cells (all‐PSCs). However, the electron mobilities (μes) of most PAs are inferior to those of their small molecule acceptor (SMA) counterparts. Herein, the authors design a new series of the polymerized SMA‐based PAs (Y5‐A‐B), where the donating moiety (A = selenophene (Se)/biselenophene (BiSe)) and the backbone regioregularity (B = In/Mix/Out) are 2D controlled, for enhancing both the μe and PCEs. Interestingly, the effects of regioisomers on the μe and all‐PSC performance are the opposite depending on the donating unit. For the Y5‐Se‐based PAs, the PCEs increase in order of Out (7.52%) < Mix (9.33%) < In (13.38%). In contrast, for the Y5‐BiSe‐based PAs, the PCEs decrease in order of Out (10.67%) > Mix (9.58%) > In (8.52%). These opposite trends in each series originate from the different planarity and intermolecular assembly of PAs depending on the regioregularity. Thus, the Y5‐Se‐In blend exhibits the highest μe and achieves the highest PCE (13.38%) among the all‐PSCs in this study. Therefore, the authors report the importance of simultaneous engineering of the backbone building unit and regioregularity to realize high‐mobility PA and highly efficient all‐PSCs.
Challenges and Strategies of Low‐Cost Aluminum Anodes for High‐Performance Al‐Based Batteries
Authors: Jiang Min , Fu Chaopeng , Meng Pengyu , Ren Jianming , Wang Jing , Bu Junfu , Dong Anping , Zhang Jiao , Xiao Wei , Sun Baode 
Published: October 2021

AbstractThe ever‐growing market of electric vehicles and the upcoming grid‐scale storage systems have stimulated the fast growth of renewable energy storage technologies. Aluminum‐based batteries are considered one of the most promising alternatives to complement or possibly replace the current lithium‐ion batteries owing to their high specific capacity, good safety, low cost, light weight, and abundant reserves of Al. However, the anode problems in primary and secondary Al batteries, such as, self‐corrosion, passive film, and volume expansion, severely limit the batteries’ practical performance, thus hindering their commercialization. Herein, an overview of the currently emerged Al‐based batteries is provided, that primarily focus on the recent research progress for Al anodes in both primary and rechargeable systems. The anode reaction mechanisms and problems in various Al‐based batteries are discussed, and various strategies to overcome the challenges of Al anodes, including surface oxidation, self‐corrosion, volume expansion, and dendrite growth, are systematically summarized. Finally, future research perspectives toward advanced Al batteries with higher performance and better safety are presented.
Magnetic Topological Insulator Heterostructures: A Review
Authors: Liu Jieyi , Hesjedal Thorsten 
Published: October 2021

AbstractTopological insulators (TIs) provide intriguing prospects for the future of spintronics due to their large spin–orbit coupling and dissipationless, counter‐propagating conduction channels in the surface state. The combination of topological properties and magnetic order can lead to new quantum states including the quantum anomalous Hall effect that was first experimentally realized in Cr‐doped (Bi,Sb)2Te3 films. Since magnetic doping can introduce detrimental effects, requiring very low operational temperatures, alternative approaches are explored. Proximity coupling to magnetically ordered systems is an obvious option, with the prospect to raise the temperature for observing the various quantum effects. Here, an overview of proximity coupling and interfacial effects in TI heterostructures is presented, which provides a versatile materials platform for tuning the magnetic and topological properties of these exciting materials. An introduction is first given to the heterostructure growth by molecular beam epitaxy and suitable structural, electronic, and magnetic characterization techniques. Going beyond transition‐metal‐doped and undoped TI heterostructures, examples of heterostructures are discussed, including rare‐earth‐doped TIs, magnetic insulators, and antiferromagnets, which lead to exotic phenomena such as skyrmions and exchange bias. Finally, an outlook on novel heterostructures such as intrinsic magnetic TIs and systems including 2D materials is given.
Designing a Zn–Ag Catalyst Matrix and Electrolyzer System for CO2 Conversion to CO and Beyond
Authors: Lamaison Sarah , Wakerley David , Kracke Frauke , Moore Thomas , Zhou Lan , Lee Dong Un , Wang Lei , Hubert McKenzie A. , Aviles Acosta Jaime E. , Gregoire John M. , Duoss Eric B. , Baker Sarah , Beck Victor A. , Spormann Alfred M. , Fontecave Marc , Hahn Christopher , Jaramillo Thomas F. 
Published: October 2021

AbstractCO2 emissions can be transformed into high‐added‐value commodities through CO2 electrocatalysis; however, efficient low‐cost electrocatalysts are needed for global scale‐up. Inspired by other emerging technologies, the authors report the development of a gas diffusion electrode containing highly dispersed Ag sites in a low‐cost Zn matrix. This catalyst shows unprecedented Ag mass activity for CO production: −614 mA cm−2 at 0.17 mg of Ag. Subsequent electrolyte engineering demonstrates that halide anions can further improve stability and activity of the Zn–Ag catalyst, outperforming pure Ag and Au. Membrane electrode assemblies are constructed and coupled to a microbial process that converts the CO to acetate and ethanol. Combined, these concepts present pathways to design catalysts and systems for CO2 conversion toward sought‐after products.
Novel Materials for Urban Farming
Authors: Xi Lifei , Zhang Mengyuan , Zhang Liling , Lew Tedrick T. S. , Lam Yeng Ming 
Published: October 2021

AbstractScarcity of natural resources, shifting demographics, climate change, and increasing waste are four major challenges in the quest to feed the exploding world population. These challenges serve as the impetus to harness novel technologies to improve agriculture, productivity, and sustainability. Urban farming has several advantages over conventional farming: higher productivity, improved sustainability, and the ability to provide fresh food all year round. Novel materials are key to accelerating the evolution of urban farming – with their ability to facilitate controlled release of nutrients and pesticides, improved seed health, substrates with better water retention capability, more efficient recycling of agricultural waste, and precise plant health monitoring. Materials science enables environmental sustainability and higher harvest yields in urban farms. Here, Singapore is used as an example of a land‐scarce city where urban farming may be the solution for future food production. Potential research directions and challenges in urban farming are highlighted, and how material optimization and innovation drive the development of urban farming to meet national and global food demands is briefly discussed. This review serves as a guide for researchers and a reference for stakeholders of urban farms, policy makers, and other interested parties.
Advancing 2D Perovskites for Efficient and Stable Solar Cells: Challenges and Opportunities
Authors: Zhao Xiaoming , Liu Tianran , Loo Yueh‐Lin 
Published: October 2021

AbstractPerovskite solar cells (PSCs) have rapidly emerged as one of the hottest topics in the photovoltaics community owing to their high power‐conversion efficiencies (PCE), and the promise to be produced at low cost. Among various PSCs, typical 3D perovskite‐based solar cells deliver high PCE but they suffer from severe instability, which restricts their practical applications. In contrast to 3D perovskites, 2D perovskites that incorporate larger, less volatile, and generally more hydrophobic organic cations exhibit much improved thermal, chemical, and environmental stability. 2D perovskites can have different roles within a solar cell, either as the primary light absorber (2D PSCs), or as a capping layer atop a 3D perovskite absorbing layer (2D/3D PSCs). Tradeoffs between PCE and stability exist in both types of PSCs—2D PSCs are more stable but exhibit lower efficiency while 2D/3D PSCs deliver exciting efficiency but show relatively poor stability. To address this PCE/stability tradeoff, the challenges both the 2D and 2D/3D PSCs face are identified and select works the community has undertaken to overcome them are highlighted in this review. It is ended with several recommendations on how to further improve PSCs so their performance and stability can be commensurate with application requirements.
Plasmonic Amyloid Tactoids
Authors: Yuan Ye , Almohammadi Hamed , Probst Julie , Mezzenga Raffaele 
Published: October 2021

AbstractDespite their link to neurodegenerative diseases, amyloids of natural and synthetic sources can also serve as building blocks for functional materials, while possessing intrinsic photonic properties. Here, it is demonstrated that orientationally ordered amyloid fibrils exhibit polarization‐dependent fluorescence, and can mechanically align rod‐shaped plasmonic nanoparticles codispersed with them. The coupling between the photonic fibrils in liquid crystalline phases and the plasmonic effect of the nanoparticles leads to selective activation of plasmonic extinctions as well as enhanced fluorescence from the hybrid material. These findings are consistent with numerical simulations of the near‐field plasmonic enhancement around the nanoparticles. The study provides an approach to synthesize the intrinsic photonic and mechanical properties of amyloid into functional hybrid materials, and may help improve the detection of amyloid deposits based on their enhanced intrinsic luminescence.
Research Progress of Bioactive Glass and Its Application in Orthopedics
Authors: Huang Chao , Yu Min , Li Hao , Wan Xufeng , Ding Zichuan , Zeng Weinan , Zhou Zongke 
Published: October 2021

AbstractBioactive glass (BG) is a classical bone biomaterial. The main characteristics of BG that support their use in orthopedics include good osteoconductivity, osteostimulativity, degradability, and suitable mechanical strength. When implanted into the body, BG can effectively strengthen the bonding between soft and hard tissues, promote the formation of dense hydroxyapatite (HA) layer on its surface which is similar to human bone tissue, and quickly combine with bone tissue, to induce and accelerate the process of bone growth. In recent years, numerous studies have been published on the application of BG in orthopedics, and its application scope is also extensive. Here, a comprehensive and systematic literature review is conducted on the application of BG in orthopedics in various aspects including BG nanoparticles, BG nanofibers, BG scaffolds, metal ion‐loaded BG, drug and biological factor‐load BG, injectable BG‐based hydrogels/pastes, BG bone cement, BG coating, etc. Although remarkable progress has been made, numerous problems limit the clinical application of BG and need to be solved by further research.
Membrane‐Mediated Self‐Organization of Rod‐Like DNA Origami on Supported Lipid Bilayers
Authors: Khmelinskaia Alena , Franquelim Henri G. , Yaadav Renukka , Petrov Eugene P. , Schwille Petra 
Published: October 2021

AbstractOrganization of elongated particles into ordered phases on 2D surfaces and interfaces has been extensively studied during the last decades both theoretically and experimentally. For mutually repulsive particles on solid nondeformable substrates, the process is controlled only by the aspect ratio and the surface density of the adsorbed particles. The local elastic response of soft substrates to particle adhesion can drastically change the collective behavior of adsorbed rod‐like particles resulting in their self‐organization via substrate‐mediated interparticle attraction. Here, high‐speed atomic force microscopy is used to study the organization of DNA origami particles on locally responsive supported lipid bilayers (SLBs) in comparison with that on nondeformable solid mica surfaces. At high surface coverage, the aspect ratio‐dependent anisotropic phases expected for densely packed particles are observed. At intermediate and low surface densities, however, a drastically different phenomenology is observed: surprisingly strong surface‐mediated interparticle attraction of DNA origami particles is found on SLBs resulting in their self‐organization compared to their purely repulsive interaction on a mica surface. The formation of organized aggregates of elongated DNA origami particles on SLBs is explained by exceptionally strong nanoparticle adhesion to the membrane that responds with a local deformation in spite of the presence of the solid support.
Facile Bioprinting Process for Fabricating Size‐Controllable Functional Microtissues Using Light‐Activated Decellularized Extracellular Matrix‐Based Bioinks
Authors: Kang Byeongmin , Park Yejin , Hwang Dong Gyu , Kim Donghwan , Yong Uijung , Lim Khoon S. , Jang Jinah 
Published: October 2021

AbstractThe concept of microtissues has evolved to adapt to the generation of human tissue analogs that mimic physiologically relevant morphological and functional features. These microtissues can provide an in vitro testing platform for the development of advanced therapeutic options. Optimizing the manufacturing process of biomaterials brings several great benefits to achieve the desired mechanical, chemical, and biological properties for tissue modeling. Hence, 3D bioprinting technology has been utilized to fabricate functional microtissues. However, current microtissue bioprinting systems still require a cumbersome and time‐consuming task, such as washing, which renders it difficult to maintain the shape of intact constructs, thereby resulting in inappropriate tissue morphogenesis. To overcome this limitation, a single‐step bioprinting method is developed easier and more versatile for microtissue production based on a dual‐crosslinkable decellularized extracellular matrix with ruthenium/sodium persulfate (dERS). The developed method enables the fabrication of spheroidal and tubular microstructures into a medium chamber, followed by the immediate culturing of printed structures without multiple postprocesses. The structural characteristics can be controlled by adjusting the printing parameters. Each dERS‐based microtissue promotes tissue maturation and exhibits biofunctional attributes. These results suggest that the developed method may enable the simultaneous achievement of adequate print fidelity and tissue functionality.
Organic Electroplated Luminescent Microarrays up to 2800 ppi toward Near‐Eye Displays via Diffusion‐Weakened Boundary Effects
Authors: Wang Rong , Liang Yiqian , Zhao Manlin , Chen Zhihua , Zhou Lei , Wang Lei , Yu Gang , Liu Linlin , Xie Zengqi , Peng Junbiao , Cao Yong 
Published: October 2021

AbstractThe quality of high‐resolution luminescent films is key for high‐definition and near‐eye displays, but is limited by the apparent boundary effects at sub‐micrometer scales, such as boundary quenching in inorganic light‐emitting diodes and the coffee ring effect in inkjet printing. This study demonstrates that the electroplating of electrified electrode microarrays is not limited by boundary effects, enabling the deposition of luminescent dyes as high‐quality films with uniform and smooth morphologies as well as strong electroluminescence. As radial diffusion is the key to boundary effect in electroplating technology, small pixels tend to weaken the boundary effects and ease the overlap of diffusion layers. When the pixel size is lower than the critical value, the boundary effects can be eliminated. The smallest pixel width attempted is 3 µm, and prototype devices of monochrome and red‐green‐blue‐colored pixel arrays are successfully fabricated on glass and flexible backplanes without bad pixels and lines, indicating the high potential of the electroplating technique to achieve high‐resolution and immersive virtual reality for fine displays.
Palladium‐Catalyzed Annulation of Arylbenzamides with Diaryliodonium Salts
Authors: Pan Cheng , Wang Limin , Han Jianwei 
Published: October 2021

AbstractBy using diaryliodonium salts, a cylization has been accomplished in the synthesis of N‐aryl phenanthridinone derivatives via a cascade of ortho‐arylation and Csp2‐N bond formation in the presence of palladium catalyst. The reaction exhibits a broad compatibility of readily available N‐arylnaphthamides.magnified image
Chiral Phosphoric Acid‐Catalyzed Enantioselective Synthesis of Pyrazole‐Based Unnatural α‐Amino Acid Derivatives
Authors: Woldegiorgis Alemayehu Gashaw , Han Zhao , Lin Xufeng 
Published: October 2021

AbstractAn enantioselective synthesis of unnatural pyrazole‐based α‐chiral amino acid derivatives from the asymmetric reaction of N‐aryl‐5‐aminopyrazoles with β,γ‐alkynyl‐α‐imino esters using a chiral spirocyclic phosphoric acid catalyst was developed. Using the established methodology, various pyrazole‐based α‐amino acid derivatives with tetrasubstituted carbon stereocenters were obtained in 67–98% yields and with 73–99% enantioselectivities. The NH2 functionality in the corresponding products enables further transformations to a chiral thiourea and a lactam.magnified image
Asymmetric Conjugate Addition of 3‐Hydroxychromen‐4‐Ones to Electron‐Deficient Olefins Catalyzed by Recyclable C2‐Symmetric Squaramide
Authors: Kovalevsky Ruslan A. , Kucherenko Alexander S. , Korlyukov Alexander A. , Zlotin Sergei G. 
Published: October 2021

AbstractThe readily scalable asymmetric synthesis of the chiral chromone derivatives functionalized at position 2 via electrophilic enantioselective olefination of the chromone core with nitroolefins and ß,γ‐unsaturated α‐ketoesters in the presence of simple C2‐symmetric tertiary amine‐squaramide catalyst was developed. The reaction products were obtained in 80–99% yield with 89–99% ee in 95% EtOH. The absolute configurations of the synthesized chromone derivatives were unambiguously established by transformation of compound (R)‐3 aa to known methyl (R)‐β‐nitro‐α‐phenylpropionate and by the single crystal XRD analysis of compounds (R,S)‐5 aa and (R,S)‐5 ab. Catalyst V poorly soluble in common organic solvents could be easily separated from the reaction mixture and reused up to 10 catalytic cycles. Catalytic hydrogenation and esterification reactions of the synthesized compounds were carried out to demonstrate synthetic potential of the developed procedure.magnified image
Enzyme Access Tunnel Engineering in Baeyer‐Villiger Monooxygenases to Improve Oxidative Stability and Biocatalyst Performance
Authors: Seo Eun‐Ji , Kim Myeong‐Ju , Park So‐Yeon , Park Seongsoon , Oh Deok‐Kun , Bornscheuer Uwe , Park Jin‐Byung 
Published: October 2021

AbstractHydrogen peroxide is involved in a variety of enzyme catalysis as an oxidant or toxic by‐product. Thereby, attenuation of the H2O2‐driven oxidative stress is one of the key issues for preparative biocatalysis. Here, a rational approach to improve the robustness of enzymes, in particular, Baeyer‐Villiger monooxygenases (BVMOs) against H2O2 was investigated. The enzyme access tunnels, which may serve as exit paths for H2O2 from the active site to the bulk, were predicted by using the CAVER and/or protein energy landscape exploration (PELE) software for the phenylacetone monooxygenase variant (PAMO_C65D) from Thermobifida fusca and the BVMO from Pseudomonas putida KT2440. The amino acid residues, which are susceptible to oxidation by H2O2 (e. g., methionine and tyrosine) and located in vicinity of the predicted H2O2 migration paths, were substituted with less reactive or inert amino acids (e. g., leucine and isoleucine). This led to design of the H2O2‐resistant enzyme variants, which became robust biocatalysts for synthetic applications. For instance, the H2O2‐resistant P. putida BVMO reached turnover numbers of 4,100 for the BV oxygenation of 4‐decanone, which is 2.8‐fold greater than the parent enzyme. Moreover, the H2O2‐resistant P. putida BVMO allowed 2‐fold enhancement in titer of 9‐(nonanoyloxy)nonanoic acid (8) formation in a cascade fatty acid biotransformation. Therefore, it was assumed that the CAVER/PELE‐based H2O2 migration path engineering represents an efficient rational design approach to improve not only oxidative stability but also biotransformation performance of the H2O2‐forming or utilizing enzymes (e. g., BVMOs, oxidases, and peroxidases).magnified image
The Journey of Alternative and Sustainable Substitutes for “Single‐Use” Plastics
Authors: Wani Waseem A. , Pathan Shabnam , Bose Suryasarathi 
Published: October 2021

AbstractPlastics are excellent materials owing to their multipurpose uses. They are simple synthetic macromolecules with versatile properties. On the disposal front, nearly 90% of the plastic products are discarded only after a single use, which keeps accumulating, impacting both terrestrial and marine life. About 6.3 billion tonnes of plastic waste have accumulated worldwide from the time of the plastic revolution. Around 79% of plastic waste amasses in landfills every year, and 2.41 million tonnes of the waste enters oceans. The accumulation of this waste poses harmful threats to the environment and flora and fauna of land and aquatic habitats. To keep a check on the generation and collection of plastic waste, the utilization of alternative materials developed from biodegradable polymers as substitutes to plastics seems quite sound. The present perspective highlights single use plastic's (SUP) challenges and the importance of biodegradable polymers as possible substitutes to SUPs. The scope of different biodegradable polymers and their suitability for developing alternative materials to SUPs is discussed. In addition, the current market status of alternative materials produced from biodegradable polymers is described. Finally, a perspective on the future of biodegradable polymers as substitutes to plastics for envisaging a green world is outlined.