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science China Materials 2024年第3期67卷 796-803页

作者：赵秋玉王静庄严宫磊张薇宁樊唯镏鲁振张永政藤田武志张平薛其坤 School of Physics and Physical Engineering Qufu Normal UniversityQufu 273165China School of Chemistry and Chemical Engineering Shandong UniversityJinan 25010China Institute of Physics Chinese Academy of SciencesBeijing 100190China Advanced Institute for Materials Research Tohoku UniversitySendai 980-8577Japan School of Environmental Science and Engineering Kochi University of TechnologyKami 782-8502Japan

由于单金属Bi在CO_(2)还原反应(CO_(2)RR)中效率较低,通过表面工程复合材料提高电导率和产率是一种有吸引力的方法.在此,我们重构了在三维纳米孔铜结构中的原位生长金属Bi纳米颗粒.得益于三维纳米多孔导电网络和Cu与Bi之间的强相互作用,... 详细信息

由于单金属Bi在CO_(2)还原反应(CO_(2)RR)中效率较低,通过表面工程复合材料提高电导率和产率是一种有吸引力的方法.在此,我们重构了在三维纳米孔铜结构中的原位生长金属Bi纳米颗粒.得益于三维纳米多孔导电网络和Cu与Bi之间的强相互作用,Bi@np-Cu费米能级向上移动,表现出优异的电催化二氧化碳还原性能.Bi@np-Cu在-0.97 V的电位下具有97.7%的甲酸法拉第效率,电流密度为82 mA cm^(-2).重要的是,该催化剂在连续催化反应40 h后仍能实现超过90%的法拉第效率.DFT计算表明,np-Cu有效地调节了Bi的电子态,优化了中间吸附能,从而提高了Bi的本征活性.这项工作为纳米多孔金属在催化中的应用提供了一个新视角.

关键词： 3D nanoporous CO_(2)RR Bi nanoparticle electrocatalysis reconstruction

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The issues on the commercialization of perovskite solar cells

Materials Futures

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Materials Futures 2024年第2期3卷 1-35页

作者： Lixiu Zhang Yousheng Wang Xiangchuan Meng Jia Zhang Pengfei Wu Min Wang Fengren Cao Chunhao Chen Zhaokui Wang Fu Yang Xiaodong Li Yu Zou Xi Jin Yan Jiang Hengyue Li Yucheng Liu Tongle Bu Buyi Yan Yaowen Li Junfeng Fang Lixin Xiao Junliang Yang Fuzhi Huang Shengzhong Liu Jizhong Yao Liangsheng Liao Liang Li Fei Zhang Yiqiang Zhan Yiwang Chen Yaohua Mai Liming Ding Center for Excellence in Nanoscience(CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication(CAS)National Center for Nanoscience and TechnologyBeijing 100190People’s Republic of China Institute of New Energy Technology College of Information Science and TechnologyJinan UniversityGuangzhou 510632People’s Republic of China Institute of Polymers and Energy Chemistry(IPEC) Nanchang UniversityNanchang 330031People’s Republic of China School of Information Science and Technology Fudan UniversityShanghai 200433People’s Republic of China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072People’s Republic of China School of Physical Science and Technology Soochow UniversitySuzhou 215006People’s Republic of China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123People’s Republic of China Institute of optoelectronics Fudan UniversityShanghai 200433People’s Republic of China College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123People’s Republic of China School of Physics and Electronic Science East China Normal UniversityShanghai 200241People’s Republic of China State Key Laboratory for Artificial Microstructure and Mesoscopic Physics Department of PhysicsPeking UniversityBeijing 100871People’s Republic of China College of Biophotonics South China Normal UniversityGuangzhou 510631People’s Republic of China School of Materials Science and Engineering Beijing Institute of TechnologyBeijing 100081People’s Republic of China School of Physics and Electronics Central South UniversityChangsha 410083People’s Republic of China School of Materials Science and Engineering Shaanxi Normal UniversityXi’an 710119People’s Republic of China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China Microquanta semiconductor Hangzhou 311121People’s Republic of China

Perovskite solar cells have aroused a worldwide research upsurge in recent years due to their soaring photovoltaic performance,ease of solution processing,and low *** power conversion efficiency record is constantly being broken and has recently reached 26.1%in the lab,which is comparable to the established photovoltaic technologies such as crystalline silicon,copper indium gallium selenide and cadmium telluride(CdTe)solar ***,perovskite solar cells are standing at the entrance of industrialization,where huge opportunities and risks ***,towards commercialization,challenges of up-scaling,stability and lead toxicity still remain,the proper handling of which could potentially lead to the widespread adoption of perovskite solar cells as a low-cost and efficient source of renewable *** review gives a holistic analysis of the path towards commercialization for perovskite solar cells.A comprehensive overview of the current state-of-the-art level for perovskite solar cells and modules will be introduced first,with respect to the module efficiency,stability and current status of *** will then discuss the challenges that get in the way of commercialization and the corresponding strategies to address them,involving the upscaling,the stability and the lead toxicity *** into the future direction of commercialization of perovskite photovoltaics was also provided,including the flexible perovskite cells and modules and perovskite indoor ***,the future perspectives towards commercialization are put forward.

关键词： commercializations perovskite solar cells state-of-the-art level challenges and perspectives indoor photovoltaics

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Generative artificial intelligence for computational chemistry: a roadmap to predicting emergent phenomena

arXiv

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arXiv 2024年

作者： Tiwary, Pratyush Herron, Lukas John, Richard Lee, Suemin Sanwal, Disha Wang, Ruiyu Department of Chemistry and Biochemistry Institute for Physical Science and Technology University of Maryland College Park20742 United States University of Maryland Institute for Health Computing Bethesda20852 United States Biophysics Program Institute for Physical Science and Technology University of Maryland College Park20742 United States Department of Physics Institute for Physical Science and Technology University of Maryland College Park20742 United States

The recent surge in Generative Artificial Intelligence (AI) has introduced exciting possibilities for computational chemistry. Generative AI methods have made significant progress in sampling molecular structures across chemical species, developing force fields, and speeding up simulations. This Perspective offers a structured overview, beginning with the fundamental theoretical concepts in both Generative AI and computational chemistry. It then covers widely used Generative AI methods, including autoencoders, generative adversarial networks, reinforcement learning, flow models and language models, and highlights their selected applications in diverse areas including force field development, and protein/RNA structure prediction. A key focus is on the challenges these methods face before they become truly predictive, particularly in predicting emergent chemical phenomena. We believe that the ultimate goal of a simulation method or theory is to predict phenomena not seen before, and that Generative AI should be subject to these same standards before it is deemed useful for chemistry. We suggest that to overcome these challenges, future AI models need to integrate core chemical principles, especially from statistical mechanics. © 2024, CC BY.

关键词： Generative adversarial networks

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Zn-ion ultrafluidity via bioinspired ion channel for ultralong lifespan Zn-ion battery

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National science Review 2024年第8期11卷 253-263页

作者： Fan Zhang Ting Liao Dong-Chen Qi Tony Wang Yanan Xu Wei Luo Cheng Yan Lei Jiang Ziqi Sun School of Chemistry and Physics Queensland University of Technology School of Mechanical Medical and Process Engineering Queensland University of Technology Centre for Materials Science Queensland University of Technology Central Analytical Research Facility Queensland University of Technology State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and Chemistry Chinese Academy of Sciences School of Mathematical and Physical Sciences University of Technology Sydney

Rechargeable aqueous Zn-ion batteries have been deemed a promising energy storage ***,the dendrite growth and side reactions have hindered their practical ***,inspired by the ultrafluidic and K+ion-sieving flux through enzyme-gated potassium channels（KcsA） in biological plasma membranes,a metal-organic-framework（MOF-5） grafted with-ClO4groups（MOF-ClO4） as functional enzymes is fabricated to mimic the ultrafluidic lipid-bilayer structure for gating Zn2+'on' and anions 'off'*** MOF-ClO4achieved perfect Zn2+/SO42-selectivity（～10）,enhanced Zn2+transfer number(tZn2+=0.88) and the ultrafluidic Zn2+flux(1.9×10-3vs.1.67 mmol m-2s-1for KcsA).The symmetric cells based on MOF-ClO4achieve a lifespan of over 5400 h at 10 mA cm-2/20 mAh ***,the performance of the PMCl-Zn//V2O5pouch cell keeps 81% capacity after 2000 cycles at 1 A *** regulated ion transport,by learning from a biological plasma membrane,opens a new avenue towards ultralong lifespan aqueous batteries.

关键词： aqueous Zn-ion battery ultrafluidic bioinspired electrode dendrite-free Zn deposition

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TiO2 Hole Transport Layer Incorporated in a Thermally Evaporated Sb2Se3 Photoelectrode Exhibiting Low Onset Potential for Photoelectrochemical Applications

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Energy and Fuels 2024年第17期38卷 16936-16948页

作者： Xavier, Thatheyus Peter Piraviperumal, Malar Kuo, Chih-Yu Govindasamy, Mani Thinfilm Photovoltaics Laboratory Department of Physics and Nanotechnology SRM Institute of Science and Technology Tamil Nadu Kattankulathur603203 India Department of Chemical Engineering & Biotechnology National Taipei University of Technology Taipei City10608 Taiwan Research Center for Intelligence Medical Devices Ming Chi University of Technology New Taipei City243303 Taiwan Department of Research and Innovation Saveetha School of Engineering SIMATS Chennai602105 India Taipei10608 Taiwan International Ph.D. Program in Innovative Technology of Biomedical Engineering and Medical Devices Ming Chi University of Technology New Taipei City243303 Taiwan

Developing cost-effective photoelectrodes with a low band gap in the NIR-visible regions remains a challenge to achieve effective hydrogen production. We report the details of superstrate-configured photocathodes, consisting of antimony selenide (Sb2Se3) light absorbing layers with titanium dioxide (TiO2) as a hole transport layer, exhibiting the capability for hydrogen evolution with broad range light absorption enabled by the low band gap value of ∼1.2 eV of Sb2Se3. Strong anisotropy is a significant characteristic property of Sb2Se3, allowing superior electrical transportation along the [hkl] crystallographic orientation, which is obtained via close space evaporation of presynthesized bulk material at a growth temperature of 250 °C, over the solution-processed TiO2 film on a fluorine-doped tin oxide (FTO) substrate. The superstrate-configured FTO/TiO2/Sb2Se3 photocathode exhibited a photocurrent density of 100 μA cm-2 at −0.3 V vs RHE in 0.5 M H2SO4 under 1 sun illumination. To further improve photocurrent density, Pt as a cocatalyst was deposited over Sb2Se3 that led to enhanced photocurrent to 3 mA cm-2 at −0.3 V vs RHE in 0.5 M H2SO4 under 1 sun illumination. Despite the relatively lower photocurrent observed, which resulted due to a large conduction band offset (ΔECB = 0.99 eV) of the TiO2/Sb2Se3 interface in a superstrate configuration, a significantly lower onset potential of −0.1 V vs RHE was observed. The results are encouraging due to the low band gap of Sb2Se3, photocorrosion stability, and straightforward fabrication, which is expected to assist for significant outcomes. © 2024 American chemical Society.

关键词： Titanium dioxide

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Solid-state stepwise temperature-programmable synthesis of bioinspired Fe-N-C oxygen reduction electrocatalyst featuring Fe-N_(5)configuration

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Nano Research 2025年第3期18卷 654-665页

作者： Wei Sang Somboon Chaemchuen Longyang Zhang Zechen Wang Xingchuan Li Cocoro Andrew Nagasaka Mo Xiong Naoki Ogiwara Cheng Chen Zhao Wang Jian Zhang Francis Verpoort Shichun Mu Zongkui Kou Tingting Wang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Department of Basic Science School of Arts and SciencesThe University of TokyoKomabaMeguro-kuTokyo 153-8902Japan MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter School of PhysicsXi’an Jiao tong UniversityXi’an 710049China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China Department of Chemical Engineering Faculty of EngineeringMahidol UniversityNakhon Pathom 73170Thailand School of Mathematical&Physical Sciences Wuhan Textile UniversityWuhan 430200China Joint Institute of Chemical Research(FFMiEN) Peoples Friendship University of Russia(RUDN University)6 Miklukho-Maklaya Str.117198 MoscowRussia National Research Tomsk Polytechnic University Lenin Avenue 30634050 TomskRussia Hubei Key Laboratory of Ferro &Piezo-electric Materials and DevicesFaculty of Physics and Electronic SciencesHubei UniversityWuhan 430062China School of Chemistry and Chemical Engineering Hainan UniversityHaikou 57022China

The bioinspired Fe-N-C features an asymmetric Fe-N_(5)configuration to produce active metal-oxygen intermediates by introducing axial N ligand into a symmetric Fe-N_(4) structure,enabling highly active oxygen reduction reaction(ORR).However,the artificial creation of active Fe-N_(5)configuration with a direct,facile and green method has been rarely developed yet,as current techniques involve complex processes and costly ***,we advance a novel solid-state stepwise temperature-programmable(SST)route to directly produce bioinspired Fe-N_(5)-*** then demonstrate that such a Fe-N_(5)-C exhibits a quite higher half-wave potential(0.92 V)with 22-fold faster ORR kinetics(15.6 mA·cm^(−2)@0.85 V)over that of the commercial Pt/C ***,we perform density functional theory(DFT)to find that the Fe is discharged with an extra 0.1 e^(−)through the axially coordinate N ligand,which significantly enhances the ability to activate O_(2) and enables an easier desorption of the crucial intermediate ^(*)OH on the Fe-N_(5)configuration over the conventional Fe-N_(4) structure.

关键词： single atom catalysts Fe-N_(5)coordination solvent-free synthesis oxygen reduction reaction(ORR) metal-air battery

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Oil-polluted water purification via the carbon-nanotubes-doped organohydrogel platform

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Nano Research 2022年第6期15卷 5653-5662页

作者： Xuetao Xu Xizi Wan Haonan Li Yikai Zhang Wen He Shuli Wang Miao Wang Xu Hou Shutao Wang CAS Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China College of Chemistry and Chemical Engineering Xiamen UniversityXiamen 361005China College of Materials Xiamen UniversityXiamen 361005China College of Physical Science and Technology Xiamen UniversityXiamen 361005China University of Chinese Academy of Sciences Beijing 100049China

Solar-driven evaporators are promising for tackling freshwater scarcity but still challenged in simultaneously realizing comprehensive performances at one platform for sustainable and efficient application in real-world environments,such as stablefloating,scalability,salt-resistance,efficient vaporization,and anti-oil-fouling ***,we design a hybrid organohydrogel evaporator to achieve the enduring oil contamination repulsion with maintaining accelerated evaporation process,and integrate capacities of ultra-stable floating,hindered salt-crystallization,large-scale fabrication for practical purification of seawater and polluted *** raised water surface surrounding evaporators,induced by low density of organogel-phase,results in oil contamination resistance through the lateral capillary repulsion ***,the organogel-phase containing photo-thermal carbon-nanotubes with low thermal capacity and conduction can form locally confined hot dots under solar irradiation and reduce heat dissipation on heating excessive ***,based on this approach,accelerated long-term practical purification of oilcontaminated solutions without any extra disposal is *** other properties of ultra-stable floating,large-scale fabrication,and anti-salt crystallization,these innovative organohydrogel evaporators open pathways for purifying oil-slickpolluted water via interfacial evaporation and are anticipated accelerating industrialization of efficient and sustainable solar-driven water purification.

关键词： solar-driven evaporation organohydrogel anti-oil-fouling thermal management ultra-stable floating

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Planar-symmetry-breaking induced antisymmetric magnetoresistance in van der Waals ferromagnet Fe_(3)GeTe_(2)

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Nano Research 2022年第3期15卷 2531-2536页

作者： Ping Liu Caixing Liu Zhi Wang Meng Huang Guojing Hu Junxiang Xiang Chao Feng Chen Chen Zongwei Ma Xudong Cui Hualing Zeng Zhigao Sheng Yalin Lu Gen Yin Gong Chen Kai Liu Bin Xiang Hefei National Laboratory for Physical Sciences at the Microscale Department of Materials Science&EngineeringCAS Key Lab of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei 230026China School of Science Nanjing University of Posts and TelecommunicationsNanjing 210023China Anhui Key Laboratory of Condensed Matter Physics at Extreme Conditions High Magnetic Field LaboratoryChinese Academy of SciencesHefei 230031China Sichuan New Materials Research Center Institute of Chemical MaterialsCAEPChengdu 610200China Anhui Laboratory of Advanced Photon Science and Technology University of Science and Technology of ChinaHefei 230026China Physics Department Georgetown UniversityWashingtonDC 20057USA

Recently discovered magnetic van der Waals(vdW)materials provide an ideal platform to explore low-dimensional magnetism and spin *** vdW interaction nature opens up unprecedented opportunities to build vertically stacked heterostructures with novel properties and *** engineering the planar structure as an alternative degree of freedom,herein we demonstrate an antisymmetric magnetoresistance(MR)in a vdW Fe_(3)GeTe_(2)flake with a step terrace that breaks the planar *** antisymmetric MR originates from a sign change of the anomalous Hall effect and the continuity of the current transport near the boundary of magnetic domains at the step edge.A repeatable domain wall due to the unsynchronized magnetization switching is responsible for this sign *** interpretation is supported by the observation of field-dependent domain switching,and the step thickness,temperature,and magnetic field orientation dependent *** work opens up new opportunities to encode magnetic information by controlling the planar domain structures in vdW magnets.

关键词： 2D magnetism Fe_(3)GeTe_(2) planar structure engineering antisymmetric magnetoresistance

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Unsaturated cobalt single-atoms stabilized by silanol nests of zeolites for efficient propane dehydrogenation

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Chinese Journal of Catalysis 2025年第5期72卷 323-333页

作者： Liwen Guo Dao Shi Tianjun Zhang Yanhang Ma Guodong Qi Jun Xu Qiming Sun Innovation Center for Chemical Science College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State Key Laboratory of New Pharmaceutical Preparations and Excipients College of Chemistry and Materials ScienceHebei UniversityBaoding 071002HebeiChina School of Physical Science and Technology&Shanghai Key Laboratory of High-resolution Electron Microscopy ShanghaiTech UniversityShanghai 201210China National Center for Magnetic Resonance in Wuhan State Key Laboratory Magnetic Resonance and Atomic Molecular PhysicsWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071HuebiChina

Propane dehydrogenation(PDH)has emerged as a key on-purpose technology for the production of propylene,but it often depends on toxic chromium and expensive platinum catalysts,highlighting the need for environmentally friendly and cost-effective *** this study,we developed a facile impregnation method to fabricate unsaturated Co single-atoms with a tricoordinated Co_(1)O_(3)H_(x) structure by regulating silanol nests in purely siliceous Beta *** PDH catalytic tests and characterizations revealed a positive correlation between the presence of silanol nests and enhanced catalytic ***,the unsaturated Co single-atoms exhibited a carbon deposition rate more than an order of magnitude slower than that of Co ***,the optimized Co_(0.3%)/deAl-meso-Beta catalyst achieved a record-high propylene formation rate of 21.2 mmol_(C3H6) g_(cat)^(-1) h^(-1),with an exceptional propylene selectivity of 99.1%at 550℃.Moreover,the Co_(0.3%)/deAl-meso-Beta catalyst demonstrated excellent stability,with negligible deactivation after 5 consecutive regeneration *** study emphasizes the pivotal role of silanol nests of zeolites in stabilizing and modulating the coordination environment of metallic active sites,providing valuable insights for the design of high-activity,high-stability,and low-cost PDH catalysts.

关键词： Propane dehydrogenation Unsaturated cobalt Single-atoms Silanol nest Zeolite

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High-Pressure Synthesis of Quadruple Perovskite Oxide CaCu3Cr2Re2O12 with a High Ferrimagnetic Curie Temperature

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Inorganic Chemistry 2024年第7期63卷 3499-3505页

作者： Zhang, Jie Liu, Zhehong Ye, Xubin Wang, Xiao Lu, Dabiao Zhao, Haoting Pi, Maocai Chen, Chien-Te Chen, Jeng-Lung Kuo, Chang-Yang Hu, Zhiwei Yu, Xiaohui Zhang, Xueqiang Pan, Zhao Long, Youwen Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing100049 China College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Sciences Beijing100049 China Songshan Lake Materials Laboratory Guangdong Dongguan523808 China National Synchrotron Radiation Research Center Hsinchu30076 Taiwan Department of Electrophysics National Yang Ming Chiao Tung University Hsinchu30010 Taiwan Max Planck Institute for Chemical Physics of Solids Dresden01187 Germany

An AA’3B2B’2O12-type quadruple perovskite oxide of CaCu3Cr2Re2O12 was synthesized at 18 GPa and 1373 K. Both an A- and B-site ordered quadruple perovskite crystal structure was observed, with the space group Pn-3. The valence states are verified to be CaCu32+Cr23+Re25+O12 by bond valence sum calculations and synchrotron X-ray absorption spectroscopy. The spin interaction among Cu2+, Cr3+, and Re5+ generates a ferrimagnetic transition with the Curie temperature (TC) at about 360 K. Moreover, electric transport properties and specific heat data suggest the presence of a half-metallic feature for this compound. The present study provides a promising quadruple perovskite oxide with above-room-temperature ferrimagnetism and possible half-metallic properties, which shows potential in the usage of spintronic devices. © 2024 American chemical Society.

关键词： Copper compounds

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