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Carbon Energy 2024年第4期6卷 164-221页

作者： Huilin Hou Gang Shao Yang Wang Wai‐Yeung Wong Weiyou Yang Institute of Micro/Nano Materials and Devices Ningbo University of TechnologyNingboChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhouChina Department of Applied Biology and Chemical Technology and Research Institute for Smart Energy The Hong Kong Polytechnic UniversityHong KongChina

Conversion of solar energy into H2 by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.

关键词： hydrogen photoanode photoelectrochemical substrates water splitting

An approach of the internal friction-dependent temperature changes for conventional and pure biogenic lubricating greases

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Friction 2024年第4期12卷 780-795页

作者： Leif AHME Erik KUHN MiguelÁngel DELGADO department of Mechanical Engineering and Production Management Hamburg University of Applied SciencesHamburg 20099Germany department of chemical Engineering Research in Product Technology and Chemical Processes(Pro2TecS)University of HuelvaHuelva 21071Spain

This work investigated the temperature changes inside the bulk of lubricating greases under controlled high-shear stress conditions(250-500 s-1).For this purpose,a newly developed temperature-measuring cell called Calidus was successfully tested.The temperature changes(ΔT)have been related to the greases'components(thickener,base oil-type,and composition)and the structural degradation of the lubricating greases.Furthermore,a theoretical approach was proposed for calculating the internal temperature change of lubricating greases during shear stress.All greases showed an internal temperature profile characterised by a sudden rise inΔT within the first 4 h from starting the test and subsequentΔT decay until it reaches the steady state value.Furthermore,it was found that greases C1 and C5,formulated with lithium and calcium soap,respectively,with different soap content(16.1 wt%and 9.7 wt%,respectively),but the same base castor oil,showed the highest value of the maximumΔT,c.a.3.2 K,and the most drastic drop ofΔT.These greases showed both the highest specific densities and heat capacities.In addition,they showed the lowest ratio of expended energies(Rtee),which means more structural degradation in the stressed grease.On the contrary,the grease C3,with 13 wt%of Li-soap but the lowest base oil's viscosity,showed the lowest maximumΔT and the temperature profile was characterised by a moderate variation ofΔT along the test.The biogenic grease B3 developed a low-temperature change in the group of pure bio-genic greases close to grease C3.

关键词： shear-induced structural degradation rheology temperature measurements lubricating greases density lubricating greases specific heat capacities

Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu department of applied Chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China MIIT Key Laboratory of Critical Materials technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen batteries.Despite extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still obscure.Here,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox process.The entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction kinetics.As a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts reported.These encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

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Journal of Energy Chemistry 2024年第7期94卷 568-576页

作者： Guntae Lim Dong Guk Kang Hyeon Gyu Lee Yen Hai Thi Tran Kihun An Junghyun Choi Kwang Chul Roh Do Youb Kim Seung-Wan Song department of chemical Engineering & applied Chemistry Chungnam National University Energy Storage Materials Center Korea Institute of Ceramic Engineering & Technology Advanced Energy Materials Research Center Korea Research Institute of Chemical Technology

Incorporation of higher content Si anode material beyond 5 wt%to Li-ion batteries (LIBs) is challenging,owing to large volume change,swelling,and solid electrolyte interphase (SEI) instability issues.Herein,a strategy of diacetoxydimethylsilane (DAMS) additive-directed SEI stabilization is proposed for a stable operation of Si-0.33FeSi2(named as Si-Fe) anode without graphite,which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate (FEC)additive and reduce a dependence on FEC.Unprecedented stable cycling performance of highly loaded(3.5 m A h cm-2) pure Si-Fe anode is achieved with 2 wt%DAMS combined with 9 wt%FEC additives under ambient pressure,yielding high capacity 1270 mA h g-1at 0.5 C and significantly improved capacity retention of 81%after 100 cycles,whereas short circuit and rapid capacity fade occur with FEC only additive.DAMS-directed robust SEI layer dramatically suppresses swelling and particles crossover through separator,and therefore prevents short circuit,demonstrating a possible operation of pure Si or Sidominant anodes in the next-generation high-energy-density and safe LIBs.

关键词： High-energy Li-ion battery Pure Si-Fe anode without graphite SEI layer Silane additive Suppressed swelling

Opto-fluidically multiplexed assembly and micro-robotics

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Light(Science & Applications) 2024年第3期13卷 544-554页

作者： Elena Erben Weida Liao Antonio Minopoli Nicola Maghelli Eric Lauga Moritz Kreysing Max Planck Institute of Molecular Cell biology and Genetics Dresden 01307Germany Center for Systems biology Dresden 01307Germany Institute of Biological and chemical Systems–Biological Information Processing.Karlsruhe Institute of technology(KIT) Eggenstein-Leopoldshafen 76344Germany department of applied Mathematics and Theoretical Physics University of CambridgeCambridge CB30WAUK

Techniques for high-definition micromanipulations,such as optical tweezers,hold substantial interest across a wide range of disciplines.However,their applicability remains constrained by material properties and laser exposure.And while microfluidic manipulations have been suggested as an alternative,their inherent capabilities are limited and further hindered by practical challenges of implementation and control.Here we show that the iterative application of laser-induced,localized flow fields can be used for the relative positioning of multiple micro-particles,irrespectively of their material properties.Compared to the standing theoretical proposal,our method keeps particles mobile,and we show that their precision manipulation is non-linearly accelerated via the multiplexing of temperature stimuli below the heat diffusion limit.The resulting flow fields are topologically rich and mathematically predictable.They represent unprecedented microfluidic control capabilities that are illustrated by the actuation of humanoid micro-robots with up to 30 degrees of freedom,whose motions are sufficiently well-defined to reliably communicate personal characteristics such as gender,happiness and nervousness.Our results constitute high-definition micro-fluidic manipulations with transformative potential for assembly,micro-manufacturing,the life sciences,robotics and optohydraulically actuated micro-factories.

关键词： manipulation fluid assembly

Inhibition of Defect-Induced Ice Nucleation, Propagation, and Adhesion by Bioinspired Self-Healing Anti-Icing Coatings

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Research 2024年第1期2023卷 237-246页

作者： Shu Tian Ruiqi Li Xinmeng Liu Jiancheng Wang Junyu Yu Sijia Xu Yunqing Tian Jing Yang Lei Zhang department of Biochemical Engineering Frontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering(MOE)School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Binzhou Institute of technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong Province 256606China

Anti-icing coatings on outdoor infrastructures inevitably suffer from mechanical injuries in numerous icing scenarios such as hailstorms,sandstorms,impacts of foreign objects,and icing–deicing cycles.Herein,the mechanisms of surface-defect-induced icing are clarified.At the defects,water molecules exhibit stronger adsorption and the heat transfer rate increases,accelerating the condensation of water vapor as well as ice nucleation and propagation.Moreover,the ice–defect interlocking structure increases the ice adhesion strength.Thus,a self-healing(at−20°C)antifreeze-protein(AFP)-inspired anti-icing coating is developed.The coating is based on a design that mimics the ice-binding and non-ice-binding sites in AFPs.It enables the coating to markedly inhibit ice nucleation(nucleation temperature<−29.4°C),prevent ice propagation(propagation rate<0.00048 cm^(2)/s),and reduce ice adhesion on the surface(adhesion strength<38.9 kPa).More importantly,the coating can also autonomously self-heal at−20°C,as a result of multiple dynamic bonds in its structure,to inhibit defect-induced icing processes.The healed coating sustains high anti-icing and deicing performance even under various extreme conditions.This work reveals the in-depth mechanism of defect-induced ice formation as well as adhesion,and proposes a self-healing anti-icing coating for outdoor infrastructures.

关键词： coating defect clarified

Recent progress in MOFs-based nanozymes for biosensing

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Nano Research 2024年第1期17卷 39-64页

作者： Imamdin Chandio Yongjian Ai Lei Wu Qionglin Liang MOE Key Laboratory of Bioorganic Phosphorus Chemistry&chemical biology Department of ChemistryLaboratory of Flexible Electronics TechnologyCenter for Synthetic and Systems BiologyTsinghua University-Peking University Joint Centre for Life SciencesTsinghua UniversityBeijing 100084China

Nanozymes are nanomaterials with enzyme-mimicking catalytic activity.Compared to natural enzymes,nanozymes show various properties such as easy to manufacture,stable,adjustable,and inexpensive.Nanozymes play key roles in biosensing,biocatalysis,and disease treatment.As an important kind of nanozymes,metal-organic framework(MOF)-based nanozymes are receiving a lot of attention due to their structural properties and composition.Rationally developing MOF with enzymes-like catalytic properties has opened new perspectives in biosensing.This review summarizes the up-to-date developments in synthesizing two-dimensional and three-dimensional MOF-based nanozymes and their applications in biosensing.Firstly,classification of nanozymes obtained by MOFs is categorized,and different properties of MOF-based nanozymes are described.Then,the distinctive applications of MOF-based nanozymes in identifying various analytes are thoroughly summarized.Finally,the recent challenges and progressive directions in this area are highlighted.

关键词： metal-organic frameworks nanozymes metal-organic framework (MOF)-based nanozymes biosensing analytes

Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels

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Chinese Journal of chemical Engineering 2024年第4期68卷 181-192页

作者： Zhourong Xiao Changxuan Zhang Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li State Key Laboratory of Metastable Materials Science and technology(MMST) Hebei Key Laboratory of Applied ChemistryCollege of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China Key Laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.

关键词： Steam reforming n-Dodecane Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)

Next-generation vaccines for substance use disorders

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Zoological Research 2024年第3期45卷 707-708页

作者： Kaixuan Wang Hongshuang Wang Xiaohui Wang Laboratory of chemical biology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchunJilin 130022China School of applied Chemistry and Engineering University of Science and Technology of ChinaHefeiAnhui 230026China

Substance use disorders(SUDs)impact an estimated 300 million people worldwide,significantly impairing both health and social functioning.These disorders are marked by an inability to regulate substance use,despite the harmful consequences.Addiction affects various neurotransmitter systems,including dopamine,serotonin,γ-aminobutyric acid(GABA),and glutamate,each of which plays a role in the reward,stress,and self-control pathways of the brain(Koob&Volkow,2016).While significant advances have been made in neuroscience,our understanding of how these neurotransmitter systems interact and contribute to addiction is still evolving.This knowledge gap represents a significant challenge in the formulation of effective treatments for SUDs.At present,the US Food and Drug Administration(FDA)has approved pharmacological treatments for alcohol,nicotine,and opioid use disorders(Vasiliu,2022);however,no such treatments have been authorized for SUDs in general,or specifically for stimulant use disorders,such as cocaine and methamphetamine addiction.Notably,the FDA has not approved any new drugs for SUD treatment in the past 40 years.

关键词： disorders treatment consequences

Rational surface charge engineering of haloalkane dehalogenase for boosting the enzymatic performance in organic solvent solutions

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Chinese Journal of chemical Engineering 2024年第1期65卷 276-285页

作者： Yin Wu Yan Sun department of Biochemical Engineering School of Chemical Engineering and Technology and Key Laboratory of Systems Bioengineering and Frontiers Science Center for Synthetic Biology(Ministry of Education)Tianjin UniversityTianjin 300350China

Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.

关键词： Surface charge engineering Organic solvent resistance Molecular dynamics simulation Haloalkane dehalogenase