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Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies

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science China Chemistry 2025年第6期 2322-2342页

作者： Mei Yi Hongmei Li Minghao Xie Panpan Li Zhaoyu Jin Guihua Yu Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China College of Materials Science and Engineering and College of Chemistry Sichuan University Materials Science and Engineering Program and Walker Department of Mechanical Engineering The University of Texas at Austin

The global nitrogen cycle holds immense importance due to its crucial role in supporting life, supplying vital nutrients for plant growth, preserving environmental balance, and enabling the proper functioning of ecosystems. However, human activities frequently disrupt this cycle, leading to the accumulation of nitrates and nitrites in water bodies. This accumulation causes environmental pollution and health risks. Traditional methods for treating nitrogen pollution, including biological, physical, and chemical approaches, have inherent limitations. In recent years, electrocatalysis has emerged as a promising and sustainable approach for nitrogen management. This technology offers superior efficiency, high selectivity, and environmental *** not only enables accurate detection of nitrogen pollutants in the environment but also facilitates their conversion into harmless nitrogen gas. Moreover, recent advancements have focused on the upcycling of nitrogen pollutants into valuable compounds,such as ammonia and urea. In this comprehensive review, we showcase the applications of electrocatalysis in sustainable nitrogen management. Specifically, we highlight its use in the sensing, removal, and upcycling of major nitrogen pollutants,including nitrate（NO3-）, nitrite（NO2-）, and nitric oxide（NO）. We discuss the use of catalysts, such as Pd alloys, Cu-based, and Fe-based materials, in electrochemical sensing and catalysis. Additionally, we explore recent advancements in the conversion of nitrogen pollutants into valuable compounds like ammonia and urea. The review also addresses current challenges and future opportunities in the field, including innovations in sensor and catalyst design, as well as large-scale treatment strategies. We anticipate that these perspectives will provide profound insights for effective nitrogen pollution control and sustainable utilization of nitrogen resources.

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Achieving high strength and large ductility in a Cr30Co30Ni30Al5Ti5 alloy through intergranular precipitation

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Journal of materials science and Technology 2025年第12期215卷 167-179页

作者： Zou, Jiawei Chen, Siyu Cheng, Pengming Ding, Jun Zhang, Chongle Zhang, Shengze Zhang, Bozhao Fu, Xiaoqian Chen, Yujie Zhao, Yuping Qi, Xu Gu, Lin Zhang, Ze Sha, Gang Yu, Qian Center of Electron Microscopy and State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou310027 China School of Materials Science and Engineering Herbert Gleiter Institute of Nanoscience Nanjing University of Science and Technology Nanjing210094 China State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Xi'an710049 China Center for Alloy Innovation and Design State Key Laboratory for Mechanical Xi'an Jiaotong University Xi'an710049 China Pico Electron Microscopy Center Innovation Institute for Ocean Materials Characterization Technology Center for Advanced Studies in Precision Instruments Hainan University Haikou570228 China Beijing National Center for Electron Microscopy and Laboratory of Advanced Materials School of Materials Science and Engineering Tsinghua University Beijing100084 China

Precipitation at grain boundaries is typically not regarded as an efficient method for strengthening materials since it can induce grain boundary embrittlement, which detrimentally affects ductility. In this research, we developed a multi-principal element alloy (MPEA) with the composition Cr30Co30Ni30Al5Ti5 (at.%), incorporating both intragranular and intergranular nanoprecipitates. Utilizing multiscale, three-dimensional, and in-situ electron microscopy techniques, coupled with computational simulations, we established that intergranular nanoprecipitation in this material plays a crucial role in enhancing strength and promoting dislocation plasticity. The structure of intergranular nanoprecipitation comprises multiple phases with varying composition and structure. Despite the diversity, the crystal planes conducive to the easy glide of dislocations are well-matched, allowing for the sustained continuity of dislocation slipping across different phase structures. Simultaneously, this structure generates an undulated stress field near grain boundaries, amplifying the strengthening effect and facilitating multiple slip and cross-slip during deformation. Consequently, it promotes the proliferation and storage of dislocations. As a result, our material exhibits a yield strength of approximately 1010 MPa and an ultimate tensile strength of around 1500 MPa, accompanied by a significant fracture elongation of 41 %. Our findings illuminate the potential for harnessing intergranular nanoprecipitation to optimize the strength-ductility trade-off in MPEAs, emphasizing the strategy of leveraging complex compositions for the design of sophisticated functional microstructures. © 2024

关键词： Ductility

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Fe single atom trigger asymmetric In-In polarized site pairs boosting near-infrared N2 photoreduction

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materials Today 2025年 86卷 96-103页

作者： Liang, Huimin Ye, Caichao Wu, Yao Li, Yezi Long, Ran Xiong, Jun Jiang, Wei Di, Jun School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research Center Nanjing University of Science and Technology Nanjing210094 China Academy for Advanced Interdisciplinary Studies & Department of Materials Science and Engineering Guangdong Provincial Key Laboratory of Computational Science and Material Design Southern University of Science and Technology Shenzhen518055 China School of Materials Science & Engineering Nanyang Technological University Singapore639798 Singapore National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience School of Chemistry and Materials Science University of Science and Technology of China Hefei230026 China Institute for Energy Research Jiangsu University Zhenjiang212013 China

Building differentiated charge distributed polarized atomic pairs may be an alternative for N2 activation. In this work, CuInS2 atomic layers with asymmetric In-In polarized site pairs are prepared by doping Fe single atoms, as proved by X-ray absorption fine structure spectroscopy, quasi in situ X-ray photoelectron spectra and calculated atomic charge distribution. The engineered Fe single atoms tuned the surface atomic charge distribution, building local polarization center to boost directional surface charge separation. The formed In-In polarized site pairs with asymmetric charge distribution creates distinct interaction with two N atoms in N2 molecule, contributing to the enhanced activation of N2. The alternating pathway is regarded as hydrogenation pathway over Fe-CuInS2 with *NNH formation as rate-determining step. The charge-redistributed surface atomic structure after engineered Fe single atoms strengthens intermediate interaction and lower the rate-determining step energy barrier. Benefiting from these features, Fe-CuInS2 exhibits excellent photocatalytic activity under near-infrared (NIR) irradiation with an ammonia synthesis rate of 94.1 μmol g−1 h−1. In comparison, the N2-NH3 conversion rate of Fe-CuInS2 under ultraviolet–visible (UV–Vis) irradiation could reach 137.4 μmol g−1 h−1, which is about 6.8 times higher than that of CuInS2. The apparent quantum efficiencies of Fe-CuInS2-2 at 380, 400, 450, 500, 550, 650, 700, 800, 850 and 1064 nm were 3.0 %, 3.3 %, 2.7 %, 2.1 %, 2.0 %, 1.5 %, 1.3 %, 0.4 %, 0.7 % and 0.6 %, respectively. © 2025 Elsevier Ltd

关键词： X ray absorption fine structure spectroscopy

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Efficient predictions of formation energies and convex hulls from density functional tight binding calculations

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Journal of materials science & Technology 2023年第10期141卷 236-244页

作者： Anshuman Kumar Zulfikhar A.Ali Bryan M.Wong Materials Science&Engineering Program University of California-RiversideRiverside92521CAUSA Department of Physics&Astronomy University of California-RiversideRiverside92521CAUSA Materials Science&Engineering Program Department of Chemical&Environmental EngineeringDepartment of Physics&Astronomyand Department of ChemistryUniversity of California-RiversideRiverside92521CAUSA

Defects in materials significantly alter their electronic and structural properties,which affect the per-formance of electronic devices,structural alloys,and functional ***,calculating all the possible defects in complex materials with conventional Density Functional Theory(DFT)can be compu-tationally *** enhance the efficiency of these calculations,we interfaced Density Functional Tight Binding(DFTB)with the Clusters Approach to Statistical Mechanics(CASM)software package for the first *** SiC and ZnO as representative examples,we show that DFTB gives accurate results and can be used as an efficient computational approach for calculating and pre-screening formation ener-gies/convex *** DFTB+CASM implementation allows for an efficient exploration(up to an order of magnitude faster than DFT)of formation energies and convex hulls,which researchers can use to probe other complex systems.

关键词： CASM DFTB DFT Formation energy Convex hull

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Recent advances on the systems metabolically engineered Pseudomonas species as versatile biosynthetic platforms for the production of polyhydroxyalkanoates

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Systems Microbiology and Biomanufacturing 2024年第2期4卷 473-499页

作者： Hye Min Song Seo Young Jo Haeyoung Lee Subeen Jeon Dohye Yun Chaerin Kim Jina Son Yu Jung Sohn Jong-Il Choi Si Jae Park Department of Chemical Engineering and Materials Science Graduate Program in System Health Science and EngineeringEwha Womans UniversitySeoul 03760Republic of Korea Department of Biotechnology and Bioengineering Chonnam National UniversityGwangju 61186Republic of Korea

Pseudomonas *** been considered one of the most promising microbial platform strains due to its versatile metabolism,enabling the valorization of waste materials into value-added chemical *** the native producer of polyhydroxyal-kanoates(PHAs),the biodegradable biopolyesters,it has been widely engineered by various metabolic engineering tools for the production of PHAs composed of short-chain-length and medium-chain-length monomers with adjustable composition from diverse carbon sources,ranging from pure sugars to crude oils and fatty *** review discusses the feasibility of Pseudomonas *** the industrial host strain and the recent advances regarding the systems metabolic engineering strategies for PHAs production in Pseudomonas sp.

关键词： Pseudomonas sp. Polyhydroxyalkanoates Systems metabolic engineering Synthetic biology Fermentation

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Anisotropic monolayer of ReX_(2)on Au foils for exploring abnormal growth behavior and electronic properties

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Nano Research 2023年第3期16卷 4197-4210页

作者： Wenzhi Quan Shuangyuan Pan Fan Zhou Yanfeng Zhang Academy for Advanced Interdisciplinary Studies Peking UniversityBeijing 100871China School of Materials Science and Engineering Peking UniversityBeijing 100871China

As an emerging class of semiconducting transition metal dichalcogenides(TMDCs),two-dimensional(2D)rhenium dichalcogenides(ReX_(2),X=S or Se)have recently aroused great research interest due to their unique anisotropic structure(1T′phase),and the related novel properties and ***,many efforts have been devoted to the controllable syntheses of high-quality monolayer or few-layer ReX_(2)flakes/films by chemical vapor deposition(CVD),wherein the metallic Au foil is found to be a unique substrate,due to the relatively strong interfacial coupling between monolayer ReX_(2)and *** the conductive nature of Au enables in situ characterizations of the as-grown ReX_(2)samples,which is essential for exploring the fundamental properties and internal growth ***,this review focuses on the recent progresses on the CVD syntheses and in situ characterizations of high-quality monolayer ReX_(2)flakes/films and their heterostructures with graphene on Au *** effects of Au foils on improving the crystal quality and inducing the growth of monolayer ReX_(2)single crystals are intensively *** crystallinity,domain morphology,atomic and electronic structures,as well as the growth behaviors of monolayer ReX_(2)flakes/films and graphene/ReX_(2)heterostructures on Au revealed by in situ characterization techniques are also *** contrasts,the growth behaviors of monolayer or few-layer ReX_(2)on insulating substrates are also ***,the potential applications of 2D ReX_(2)in new-generation electronic,optoelectronic devices,and energy-related fields are also ***,future research directions are also prospected for propelling the practical applications of 2D ReX_(2)materials in more versatile fields.

关键词： rhenium dichalcogenides(ReX_(2)) Au chemical vapor deposition scanning tunneling microscopy/spectroscopy growth behavior electronic properties

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Transfer or blockage:Unraveling the interaction between deformation twinning and grain boundary in tantalum under shock loading with molecular dynamics

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Journal of materials science & Technology 2023年第25期156卷 118-128页

作者： Z.C.Meng M.M.Yang A.H.Feng S.J.Qu F.Zhao L.Yang J.H.Yao Y.Yang Q.B.Fan H.Wang Interdisciplinary Centre for Additive Manufacturing (ICAM) School of Materials and ChemistryUniversity of Shanghai for Science and TechnologyShanghai 200093China Institute of Metal Research Chinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China School of Materials Science and Engineering Tongji UniversityShanghai 201804China Academy for Advanced Interdisciplinary Studies Southern University of Science and TechnologyShenzhen 518055China National Key Laboratory of Science and Technology on Materials Under Shock and Impact School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Institute of Technology Chongqing Innovation Center Chongqing 401135China

The interaction between{112}deformation twinning and grain boundary in coaxial polycrystalline tantalum under shock compression was studied with molecular dynamics simulation under different grain pair misorientation ... 详细信息

The interaction between{112}<111>deformation twinning and grain boundary in coaxial polycrystalline tantalum under shock compression was studied with molecular dynamics simulation under different grain pair misorientation angles(MA)and geometric compatibility factor(m’).Generally,in the coaxial polycrystal,the value of MA determines the occurrence of twin transfer(TT)or twin blockage(TB),i.e.,twin transfer occurs at MA≤29°with twin blockage *** TT,the value of m’affects the selection of twin variants.,i.e.,the twin system with a larger m’is easier to *** morphology of twin pairs is ruler-shaped and lenticular under TT and TB,respectively,with different thickening mechanisms,including grain boundary dislocation emission.

关键词： Plasticity Grain boundary Twin Atomistic simulation Tantalum

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Promoting Electrocatalytic CO_(2) Reduction to CO via Sulfur-Doped Co-N-C Single-Atom Catalyst

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Chinese Journal of Chemistry 2023年第24期41卷 3553-3559页

作者： Zhiming Wei Yuhang Liu Jie Ding Qinye He Qiao Zhang Yueming Zhai The Institute for Advanced Studies Wuhan UniversityWuhanHubei430072 China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhouJiangsu215009 China

Electrocatalytic reduction of CO_(2) to fuels and chemicals possesses huge potential to alleviate current environmental *** doping in metal-nitrogen-carbon(M-N-C)single-atom catalysts(SACs)has been found to be capable to promote the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).However,the origin of the enhanced activity is still ***,we report that sulfur-doped cobalt-nitrogen-carbon single-atom catalyst(Co1-SNC)exhibits superior CO_(2)RR performance compared to sulfur-free counterpart(Co1-NC).On the basis of in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),kinetic isotope effect(KIE)and theoretical calculation,it is demonstrated that sulfur doping can promote water activation,elevate the d-band center of Co active site,and reduce the free energy of*COOH intermediate *** work deepens the understanding of the CO_(2)RR chemistry over heteroatom-doped SACs for designing efficient CO_(2)RR processes.

关键词： Electrocatalytic CO_(2)reduction Doping Heterogeneous catalysis Single-atom catalysts ATR-SEIRAS

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Trialkylsilyl-thiophene-conjugated acceptor for efficient organic solar cells compatible with spin-coating and blade-coating technologies

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science China Chemistry 2024年第12期67卷 4184-4193页

作者： Tengfei Li Qiang Wu Ze-Fan Yao Hairui Bai Wenyan Su Rui Sun Lingxiao Tang Zhaozhao Bi Xiaojun Li Weiguo Zhu Jie Min Qunping Fan Wei Ma State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049China School of Materials Science and Engineering Xi’an University of Science and TechnologyXi’an 710054China Jiangsu Engineering Research Center of Light-Electricity-Heat Energy-Converting Materials and Applications School of Materials Science and Engineeringand Changzhou UniversityChangzhou 213164China College of Chemistry and Molecular Engineering Peking UniversityBeijing 100871China The Institute for Advanced Studies Wuhan UniversityWuhan 430072China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of Chemistry Chinese Academy of SciencesBeijing 100190China

Sidechain engineering as an efficient and convenient strategy has been widely used to optimize molecular structure of photovoltaic materials for boosting power conversion efficiency(PCE)of organic solar cells(OSCs).Herein,a new Y-series acceptor named Y-Th Si with trialkylsilyl-substituted thiophene as conjugated sidechain is *** with its parental Y6 with multiple intermolecular interactions,Y-Th Si has a unitary molecular packing due to the additional steric hindrance from twodimensional(2D)-conjugated ***,Y-Th Si shows an obviously blue-shifted absorption with an onset of~850 nm but significantly up-shifted lowest unoccupied molecular orbital energy *** the PM6:Y-Th Si pair,the spin-coating OSCs achieve a decent PCE of 14.56%with an impressively high photovoltage(V_(OC))of 0.936 *** by its high V_(OC)and narrow absorption,Y-Th Si is introduced into near-infrared absorbing binary PM6:BTP-eC9 host to construct ternary *** to the complementary absorption,optimized morphology,and minimized energy loss properties,the PM6:BTP-e C9:Y-Th Si-based OSCs offer a higher PCE of 18.34%.Moreover,our developed strategy can overcome the commonly existed PCE drop when the blade-coating towards large-scale printing is used ***,a comparable PCE of 18.34%is achieved,which is one of the best values for the blade-coating OSCs so far.

关键词： sidechain engineering organic solar cells blade-coating spin-coating power conversion efficiency

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Computing grain boundary“phase”diagrams

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Interdisciplinary materials 2023年第1期2卷 137-160页

作者： Jian Luo Department of Nanoengineering Program of Materials Science and EngineeringUniversity of California San DiegoLa JollaCaliforniaUSA

Grain boundaries(GBs)can be treated as two-dimensional(2-D)interfacial phases(also called“complexions”)that can undergo interfacial phase-like *** bulk phase diagrams and calculation of phase diagram(CALPHAD)methods serve as a foundation for modern materials science,we propose to extend them to GBs to have equally significant *** perspective article reviews a series of studies to compute the GB counterparts to bulk phase ***,a phenomenological interfacial thermodynamic model was developed to construct GB lambda diagrams to forecast high-temperature GB disordering and related trends in sintering and other properties for both metallic and ceramic *** parallel,an Ising-type lattice statistical thermodynamic model was utilized to construct GB adsorption(segregation)diagrams,which predicted first-order GB adsorption transitions and critical *** two simplified thermodynamic models emphasize the GB structural(disordering)and chemical(adsorption)aspects,***,hybrid Monte Carlo and molecular dynamics atomistic simulations were used to compute more rigorous and accurate GB“phase”*** GB diagrams of thermodynamic and structural properties were further extended to include mechanical ***,machine learning algorithms were combined with atomistic simulations to predict GB properties as functions of four independent compositional variables and temperature in a 5-D space for a given GB in high-entropy alloys or as functions of five GB macroscopic(crystallographic)degrees of freedom plus temperature and composition for a binary alloy in a 7-D *** relevant studies are also *** perspective and outlook,including two emerging fields of high-entropy grain boundaries(HEGBs)and electrically(or electrochemically)induced GB transitions,are discussed.

关键词： CALPHAD grain boundary interfacial transition phase diagram

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