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Constructing artificial mimic-enzyme catalysts for carbon dioxide electroreduction

Science China Chemistry 2022年第1期65卷 106-113页

作者： Li Li Qidong Li Xiaodong Li Shumin Wang Kai Zheng Ming Zuo Xiaolong Zu Yuan Zhao Wensheng Yan Junfa Zhu Yongfu Sun Yi Xie Hefei National laboratory for Physical Sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China engineering laboratory for Next Generation Power and energy storage Batteries Tsinghua Shenzhen International Graduate SchoolShenzhen 518055China laboratory of Advanced Materials School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Institute of energy Hefei Comprehensive National Science CenterHefei 230031China

Natural bio-enzyme catalysts usually exhibit unexpected performances for many significant reactions,which are worthy of *** we report artificial metal-sulfur-carbon(M-S-C)mimic-enzyme catalysts based on bionic *** catalysts combine metal centers and functional ligands,which realize the universal fabrication of phase and adjustable *** synthesized catalysts inherit the highly active and selective feature of bio-enzyme *** directly used for carbon dioxide electroreduction reaction,the Sn-S-C catalyst exhibits high selectivity for formate(Faradaic efficiency>95%),as well as a continuous stability over 120 h at a high current density of 740 m A cm^(-2),greatly outperforming the reported catalysts for formate *** catalytic sites and pathways are probed with in-situ Fourier transform infrared(FTIR)spectra,in-situ Raman spectra and synchrotron-radiation X-ray photoelectron *** results break the inherent conundrum that it is impossible to simultaneously realize activity and durability under high *** findings offer a versatile strategy to inherit from nature and integrate different components,thus designing efficient catalysts for various challenging reactions and energy conversions via a natural sustainable way.

关键词： carbon dioxide electroreduction universal synthesis mimic-enzyme catalysts

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Defect-rich bismuth metallene for efficient CO_(2) electroconversion

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Chinese Journal of Structural Chemistry 2023年第8期42卷 11-16页

作者： Bo-Qiang Miao Wen-Sheng Fang Bin Sun Fu-Min Li Xiao-Chen Wang Bao-Yu Xia Yu Chen Key laboratory of Macromolecular Science of Shaanxi province Shaanxi Key Laboratory for Advanced Energy DevicesSchool of Materials Science and EngineeringShaanxi Normal UniversityXi'an710062PR China School of Chemistry and Chemical engineering Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education)Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsWuhan National Laboratory for OptoelectronicsHuazhong University of Science and Technology(HUST)1037 Luoyu RdWuhan430074PR China

*** Carbon dioxide reduction(CO_(2)RR)technology has attracted much attention in recent years and can effectively decrease the greenhouse effect and simultaneously achieve chemical energy storage[1].In the electrochemical process,a large overpotential is generally required to activate inert CO_(2)molecules,resulting in the inevitable competition reaction from the hydrogen evolution reaction(HER)and consequently decreasing the faradaic efficiency of CO_(2)RR[2,3].Among various reduction products of CO_(2)RR,formate is the most prevalent product with important applications in the energy conversion and chemical *** a host of catalysts that can convert CO_(2)to formate,bismuth(Bi)-based nanomaterials are highly promising electrocatalysts for the conversion of CO_(2)to formate due to their high faradaic efficiency and good ***,the preparation method and catalytic activity of Bi-based nanomaterials still need to be further improved for industrial conversion of the CO_(2)RR.

关键词： stability. bismuth dioxide

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Synchronous activation of Ag nanoparticles and BiOBr for boosting solar-driven CO_(2)reduction

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Chinese Chemical Letters 2023年第6期34卷 252-255页

作者： Gaopeng Liu Lin Wang Bin Wang Xingwang Zhu Jinman Yang Pengjun Liu Wenshuai Zhu Ziran Chen Jiexiang Xia Key laboratory of Medicinal and Edible Plants Resources of Hainan province Hainan vocational university of Science and TechnologyHaikou 571126China School of Chemistry and Chemical engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Department of Architecture and Environment engineering Sichuan Vocational and Technical CollegeSuining 629000China

Artificial photosynthesis of valuable chemicals from CO_(2)is a potential way to achieve sustainable carbon *** CO_(2)conversion activity is still inhibited by the sluggish charge kinetics and poor CO_(2)***,Ag nanoparticles coupled Bi OBr have been constructed by in-situ photoreduction *** crafting of interface between Ag nanoparticles and Bi OBr nanosheets,achieving an ultra-fast charge *** Bi OBr semiconductor excited electrons and plasmonic Ag nanoparticles generated high-energy hot electrons synchronous accelerates the C=O double bond ***,the optimized Ag/BiOBr-2 heterostructure shows excellent CO_(2)photoreduction activity with CO production of 133.75 and 6.83μmol/g under 5 h of 300 W Xe lamp and visible light(λ>400 nm)irradiation,which is 1.51 and 2.81 folds versus the pristine Bi OBr,*** mechanism of CO_(2)photoreduction was in-depth understood through in-situ FT-IR spectrum and density functional theory *** study provides some new perspectives into efficient photocatalytic CO_(2)reduction.

关键词： Ag nanoparticles BiOBr Hot electrons Charge transfer CO_(2)photoreduction

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One‑Step Gas-Solid‑Phase Diffusion‑Induced Elemental Reaction for Bandgap‑Tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI Thin Film Solar Cells

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Nano-Micro Letters 2023年第4期15卷 261-271页

作者： Erchuang Fan Manying Liu Kangni Yang Siyu Jiang Bingxin Li Dandan Zhao Yanru Guo Yange Zhang Peng Zhang Chuantian Zuo Liming Ding Zhi Zheng Key laboratory of Micro‑Nano Materials for energy storage and Conversion of Henan province College of Chemical and Materials EngineeringInstitute of Surface Micro and Nano MaterialsXuchang UniversityXuchang 461000People’s Republic of China School of Materials Science and engineering Zhengzhou UniversityZhengzhou 450001People’s Republic of China 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

Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low ***,we developed a strategy of one-step gas-solid-phase diffusioninduced reaction to fabricate a series of bandgap-tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI bilayer films due to the atomic diffusion effect for the first *** designing and regulating the sputtered Cu/Ag/Bi metal film thickness,the bandgap of Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI could be reduced from 2.06 to 1.78 *** cells with the structure of FTO/TiO_(2)/Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI/carbon were constructed,yielding a champion power conversion efficiency of 2.76%,which is the highest reported for this class of materials owing to the bandgap reduction and the peculiar bilayer *** current work provides a practical path for developing the next generation of efficient,stable,and environmentally friendly photovoltaic materials.

关键词： Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI Elemental reaction Bandgap tuning Solar cells Gas-solid phase

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Photoexcitation induced magnetic phase transition and spin dynamics in antiferromagnetic MnPS_(3) monolayer

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npj Computational Materials 2023年第1期9卷 1246-1252页

作者： Yinlu Gao Xue Jiang Zhiyong Qiu Jijun Zhao State Key laboratory of Structural Analysis for Industrial Equipment Dalian University of Technology116024 DalianChina Key laboratory of Materials Modification by Laser Ion and Electron Beams(Dalian University of Technology)Ministry of Education116024 DalianChina Key laboratory of energy Materials and Devices(Liaoning province) School of Materials Science and EngineeringDalian University of Technology116024 DalianChina

Antiferromagnetic spin dynamics is the key issue to develop spintronic *** adopt ab initio nonadiabatic molecular dynamics with spin–orbit-coupling(SOC)to investigate photoinduced spin dynamics in an antiferromagnetic semiconductor MnPS_(3) *** doping triggers MnPS_(3) from Néel antiferromagnetic to ferromagnetic phase at an experimentally achievable electron–hole pair density of 1.11×10^(14) cm−*** phase transition can be ascribed to the light-induced mid-gap states of S-p orbitals,which lower the electron excitation energy and strengthen the SOC effect between S-p and Mn-d *** excited S-p electrons first decay to the mid-gap states due to p–p electron–phonon-coupling and then relax to the spin-down Mn-d orbitals via *** a dramatic relaxation process prolongs the photogenerated carrier lifetime up to 648 fs,providing an explanation for the unusual optoelectronic performance of MnPS_(3).The reversible switching of magnetic order via optical means gives an important clue for information storage and highly efficient photocatalysts utilizing antiferromagnetic semiconductors.

关键词： dynamics excitation monolayer

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A p-p+ homojunction enhanced hole transfer in inverted planar perovskite solar cells

A p-p+ homojunction enhanced hole transfer in inverted plana...

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第八届新型太阳能材料科学与技术学术研讨会

作者： Jian Song Liang Zhao Sheng Huang The jiangsu province engineering laboratory of high efficient energy storage technology and equipments School of Materials Science and PhysicsChina University of Mining and Technology

Here, a p-p+ homojunction is constructed on basis of NiO film to enhance hole transfer in an inverted planar perovskite solar cell. The homojunction is fabricated by NiO/Cu:NiO bilayer film, DFT calculation demonstrates the charge density difference in the two layers, which could generate a space charge region and a band bending at the junction, the result is further proved by energy level structure analysis of NiO and Cu:NiO films. This homojunction could accelerate the hole transfer and inhibit carrier recombination at the interface between hole transfer layer and perovskite layer. This work develops a new structure of hole transport layer to enhance the performance of PSCs, and also provides new ideas for design of charge transfer films.

关键词： homojunction space charge region hole transfer

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efficient Environment-friendly Lead-free Tin Perovskite Solar Cells Enabled by Incorporating 4-Fluorobenzylammonium Iodide Additives

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能源与环境材料（英文） 2023年第6期6卷 318-326页

作者： Shengli Zou Shengqiang Ren Yiting Jiang Yuanfang Huang Wenwu Wang Changlei Wang Cong Chen Xia Hao Lili Wu Jingquan Zhang Dewei Zhao College of Materials Science and engineering & Institute of New energy and Low-Carbon technology Sichuan UniversityEngineering Research Center of Alternative Energy Materials & DevicesMinistry of EducationChengdu 610065China School of Optoelectronic Science and engineering & Collaborative Innovation Center of Suzhou Nano Science and technology Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province & Key Lab of Modern Optical Technologies of Education Ministry of ChinaSoochow UniversitySuzhou 215006China

Development of tin(Sn)-based perovskite solar cells(PSCs)largely lags behind that of lead counterparts due to fast crystallization process of Sn perovskite and numerous defects in both bulk and surface of Sn perovskite ***,this work reports a facile strategy of introducing 4-fluorobenzylammonium iodide(FBZAI)as additives into Sn perovskite precursor to synergistically modulate the roles of benzylamine and fluorine in Sn-based *** of FBZAI can increase crystallinity,passivate defects,and inhibit the oxidation of Sn2+,leading to suppression of nonradiative recombination and enhancement of charge transport and collection in *** a result,the best-performing Sn-based PSC with the FBZAI additive achieves the maximum PCE of 13.85％with the enhanced fill factor of 77.8％and open-circuit voltage of 0.778 *** unencapsulated device exhibits good stability by maintaining 95％of its initial PCE after 160 days of storage.

关键词： 4-fluorobenzylammonium iodide defect passivation lead-free Sn perovskites perovskite solar cells stability

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Reconfigurable Mechanochromic Patterns into Chameleon-Inspired Photonic Papers

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Research 2022年第4期2022卷 421-433页

作者： Dongpeng Yang Yang Hu Dekun Ma Jianping Ge Shaoming Huang School of Materials and energy Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage DevicesGuangdongUniversityof TechnologyGuangzhou510006China Zhejiang Key laboratory of Alternative Technologies for Fine Chemicals Process Shaoxing UniversityShaoxing 312000China School of Chemistry and Molecular engineering Shanghai Key laboratory of Green Chemistry and Chemical Processes East China Normal UniversityShanghai200062China

Photonic crystal(PC)patterns have shown wide applications in optical devices,information encryption,anticounterfeiting,***,it is stll a great challenge to reconfigure the PC patterns once ***,a new strategy is presented to reconfigure self-recordable PC patterns by printing local patterns into the chameleon-inspired PC papers using the phase change material(PCM)as ink and then erasing the patterns in *** and high-resolution(25 and 75μm for dot and lines,respectively)patterns can be eficiently and repeatedly *** addition,the photonic patterns based on the PC paper and PCM combinations are gifted with mechanochromic characteristics and can show programmable and reversible color change under *** high melting point of the ink,nonclosely packed structures of the PC paper,and the similar solubility parameter of PC paper,PCM,and ethanol are the keys for all these *** work offers a simple,flexible,efficient way to reconfigure PC patterns with mechanochromic properties and could open up exciting applications for novel hand-operation-based anticounterfeiting and opticaldevices.

关键词： packed repeatedly printing

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In Situ Embedment of ZnS Nanocrystals in high Porosity Carbon Fibers as an Advanced Anode Material for Efcient Lithium storage

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Acta Metallurgica Sinica(English Letters) 2023年第1期36卷 167-176页

作者： Wei Wang Mingyu Guan Qinghua Wang Yangyang Chen Liang Chen Hong Yin Yucan Zhu Gangyong Li Zhaohui Hou Key laboratory of Hunan province for Advanced Carbon-Based Functional Materials School of Chemistry and Chemical EngineeringHunan Institute of Science and TechnologyYueyang 414006China Guangxi Key laboratory of Low Carbon energy Material Guangxi Normal UniversityGuilin 541004China College of Materials Science and technology Central South University of Forestry and TechnologyChangsha 410004China

ZnS is a promising material for lithium-ion battery anodes due to its abundant natural resources,simplicity of synthesis,and high theoretical lithium storage ***,it needs to be optimized for its low conductivity and volume efect during the charge–discharge *** traditional method of combining with carbonaceous materials is usually laborious,and the required sulfuration process may possibly result in the destruction of materials *** this study,hybrid materials formed by the combination of ZnS nanocrystals and high porosity carbon fbers were synthesized by one-step electrospinning using zinc diethyldithiocarbamate and polyacrylonitrile as raw materials and poly(ethylene glycol)—block-poly(propylene glycol)—block-poly(ethylene glycol)as *** method is simple and avoids the infuence of sulfuration process on the morphology of *** composite presents a specifc capacity of 592.2 mAh g^(−1) under a current density of 1 A g^(−1) after 1000 *** porous structure signifcantly decreases the difusion mean-free path of Li+and inhibits the volume efect associated with the lithium storage process of *** addition,the 3D cross-linked carbon fbers improve the conductivity of *** study can serve as an inspiration for the development of other lithium storage composites.

关键词： Electrospinning ZnS Carbon fbers Porous Lithium storage

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Dual-salt assisted synergistic synthesis of Prussian white cathode towards high-capacity and long cycle potassium ion battery

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能源化学:英文版 2023年第8期83卷 16-23,I0003页

作者： Rui Ma Zixing Wang Qingfeng Fu Wang Zhou Ying Mo Jian Tu Zhiyong Wang Peng Gao Changling Fan Jilei Liu College of Materials Science and engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangsha 410082HunanChina LI-FUN technology Corporation Limited Zhuzhou 412000HunanChina Hunan Zhongke Shinzoom technology Co. Ltd.Changsha 410082HunanChina

Prussian blue analogues(PBAs) are considered as superior cathode materials for potassium-ion batteries(PIBs) because of their three-dimensional open framework structure,high stability,and low ***,the intrinsic lattice defects and low potassium content typically results in poor rate and cycling performance,thus limited their practical *** this work,high-quality K1.64FeFe(CN)6(PW-HQ)material with less crystalline water(6.21%) and high potassium content(1.64 mol^(-1)) was successfully synthesized by a novel coprecipitation method with potassium citrate(K-CA) and potassium chloride(KCl) ***,the electrode delivers a reversible capacity of 113.1 mA h g^(-1)at the current rate of 50 mA g^(-1)with~100% coulombic ***,the electrode retained 90% reversible capacity at 500 mA g^(-1)current density after 1000 cycles,indicating only 0.01% capacity decay per ***,we have revealed that the introduction of K-CA controlled the chelating rate of Fe(Ⅱ) and the addition of KCl increased the K+content,hence improving the capacity and stability of the asprepared *** evolution and potassium storage mechanism were further investigated by detailed ex-situ X-ray diffraction and in-situ Raman measurements,which demonstrated reversible potassiation/depotassiation behavior and negligible volume change during the electrochemical *** general,this work provides an efficient strategy to eliminate water contents in Prussian blue cathode and improve its electrochemical performance,which plays a key role in promoting the industrialization of potassium ion batteries.

关键词： Potassium-ionbattery high-qualityK,FeFe(CN)s Potassiumchloride Potassiumcitrate Electrochemical properties

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