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Science China Chemistry 2022年第3期65卷 428-440页

作者： Xingchen Jiao Zexun Hu Li Li Yang Wu Kai Zheng Yongfu Sun Yi Xie Hefei National Laboratory for Physical Sciences at microscale University of Science and Technology of ChinaHefei 230026China institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

Carbon dioxide electroreduction usually suffers from low catalytic activities and debatable reaction mechanisms at present. That may be primarily ascribed to the high energy barrier for carbon dioxide activation over the conventionally fabricated catalysts and the infeasibility of traditional characterization techniques for unveiling the evolution of active sites and reactive intermediates. Two-dimensional(2 D) materials, which possess the active sites with high proportion, high activity and high uniformity, can act as ideal models to manipulate the active sites and understand structure-property relationship. In this review, we overview the boosted carbon dioxide activation by the intrinsic peculiar electronic states of 2D catalysts and the charge localization effect induced by chemical modification of two-dimensional catalysts. We also summarize the recognition of the structural evolutions for active sites in two-dimensional catalysts by means of in situ X-ray diffraction pattern and in situ X-ray absorption spectroscopy. Moreover, we emphasize the detection of the reactive intermediates on active sites in two-dimensional catalysts via in situ Raman spectroscopy and in situ Fourier transform infrared spectroscopy. Finally, we end this review with an outlook on the unresolved issues and future development of carbon dioxide electroreduction.

关键词： two-dimensional materials carbon dioxide electroreduction active site CO_(2)activation in situ characterization techniques

Industrial-current-density CO_(2)-to-formate conversion with low overpotentials enabled by disorder-engineered metal sites

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Nano Research 2022年第8期15卷 6999-7007页

作者： Zhiqiang Wang Xiaolong Zu Xiaodong Li Li Li Yang Wu Shumin Wang Peiquan Ling Yuan Zhao Yongfu Sun Yi Xie Hefei National Laboratory for Physical Sciences at microscale University of Science and Technology of ChinaHefei 230026China institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

CO_(2)electroreduction to formate is technically feasible and economically viable,but still suffers from low selectivity and high overpotential at industrial current densities.Here,lattice-distorted metallic nanosheets with disorder-engineered metal sites are designed for industrial-current-density CO_(2)-to-formate conversion at low overpotentials.As a prototype,richly lattice-distorted bismuth nanosheets are first constructed,where abundant disorder-engineered Bi sites could be observed by high-angle annular dark-field scanning transmission electron microscopy image.In-situ Fourier-transform infrared spectra reveal the CO_(2)•−*group is the key intermediate,while theoretical calculations suggest the electron-enriched Bi sites could effectively lower the CO_(2)activation energy barrier by stabilizing the CO_(2)•−*intermediate,further affirmed by the decreased formation energy from 0.49 to 0.39 eV.As a result,the richly lattice-distorted Bi nanosheets exhibit the ultrahigh current density of 800 mA·cm^(−2)with 91%Faradaic efficiencies for CO_(2)-to-formate electroreduction,and the formate selectivity can reach nearly 100%at the current density of 200 mA·cm^(−2)with a very low overpotential of ca.570 mV,outperforming most reported metal-based electrocatalysts.

关键词： CO_(2)-to-formate disorder-engineered metallic nanosheets industrial-current-density low overpotential

In-depth understanding of ionic liquid assisted perovskite film formation mechanism for two-step perovskite photovoltaics

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Journal of Energy Chemistry 2022年第10期31卷 599-606,I0015页

作者： Fei Wang Patrick Wai-Keung Fong Zhiwei Ren Hai-Lun Xia Kang Zhou Kai Wang Jiajie Zhu Xiaoxi Huang Xiao-Yuan Liu Hao Wang Yumeng Shi Haoran Lin Quanyao Zhu Gang Li Hanlin Hu Hoffman institute of Advanced Materials Shenzhen PolytechnicShenzhen 518055GuangdongChina Department of Electronic and Information Engineering Research Institute for Smart Energy(RISE)The Hong Kong Polytechnic UniversityHong Kong 999077China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 43007HubeiChina International Collaborative Laboratory of 2D Materials for optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060GuangdongChina The Hong Kong Polytechnic University Shenzhen Research institute Shenzhen 518057GuangdongChina institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an 710072ShannxiChina School of Physics Science and Engineering Tongji UniversityShanghai 200092China

Ionic liquids(ILs)have been widely applied in the one-step fabrication of perovskite with noticeable enhancement in the device performance.However,in-depth mechanism of ionic-liquid-assisted perovskite film formation is not well understood for also important two-step perovskite fabrication method,with better control of crystallization behavior.In this work,we introduced ionic liquid methylammonium formate(MAFa)into organic salt to produce perovskite film via a two-step method.Systematic investigations on the influence of MAFa on the perovskite thin film formation mechanism were performed.Ionic liquid is shown to assist lowering the perovskite formation enthalpy upon the density functional theory(DFT)calculation,leading to an accelerated crystallization process evidenced by in-situ UV-Vis absorption measurement.A gradient up-down distribution of ionic liquid has been confirmed by timeof-flight SIMS.Importantly,besides the surface passivation,we found the HCOO-can diffuse into the perovskite crystals to fill up the halide vacancies,resulting in significant reduction of trap states.Uniform perovskite films with significantly larger grains and less defect density were prepared with the help of MAFa IL,and the corresponding device efficiency over 23%was obtained by two-step process with remarkably improved stability.This research work provides an efficient strategy to tune the morphology and opto-electronic properties of perovskite materials via ionic-liquid-assisted two-step fabrication method,which is beneficial for upscaling and application of perovskite photovoltaics.

关键词： Halide vacancies Perovskite solar cells Two-step method Ionic liquid

Au/MXene based ultrafast all-optical switching

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Frontiers of physics 2023年第3期18卷 147-153页

作者： Yule Zhang Feng Zhang Bowen Du Hualong Chen S.Wageh Omar A.Al-Hartomy Abdullah G.Al-Sehemi Bin Zhang Han Zhang International Collaborative Laboratory of 2D Materials for optoelectronics Science and Technology of Ministry of Education Institute of Microscale Optoelectronics and Translational MedicineThe First Affiliated Hospital(Shenzhen Second People’s Hospital)College of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China Department of Physics Faculty of ScienceKing Abdulaziz UniversityJeddah 21589Saudi Arabia Research Center for Advanced Materials Science(RCAMS) King Khalid UniversityP.O.Box 9004Ab-ha61413Saudi Arabia

All-optical switches have arisen great attention due to their ultrafast speed as compared with electric switches.However,the excellent optical properties and strong interaction of two-dimensional(2D)material MXene show great potentials in next-generation all-optical switching.As a solution,we propose all-optical switching used Au/MXene with switching full width at half maximum(FWHM)operating at 290 fs.Compared with pure MXene,the Au/MXene behaves outstanding performances due to local surface plasmon resonance(LSPR),including broadband differential transmission,strong near-infrared on/off ratio enhancement.Remarkably,this study enhances understanding of Au/MXene based ultrafast all-optical switching red-shifted about 34 nm in comparison to MXene,validating all optical properties of Au/MXene opening the way to the implementation of optical interconnection and optical switching.

关键词： Au/MXene ultrafast all-optical switching Au/MXene carrier lifetime

Vacancy-engineering-mediated activation of excitonic transition for boosting visible-light-driven photocatalytic oxidative coupling of amines

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Nano Research 2023年第11期16卷 12655-12661页

作者： Wenxiu Liu Lei Li Peng Zhang Manqin Guan Ming Zuo Yinhua Zhao Hui Wang Xiaodong Zhang Yi Xie Hefei National Research Center for Physical Sciences at the microscale University of Science and Technology of ChinaHefei 230026China institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

The light absorption properties of semiconductor-based photocatalysts to a large extent determine the relevant catalytic performance.Traditional strategies in broadening the light absorption range are usually accompanied with unfavorable changes in redox ability and dynamics of photoinduced species that would confuse the comprehensive optimization.In this work,we propose a nontrivial excitonic transition regulation strategy for gaining sub-bandgap light absorption in low-dimensional semiconductor-based photocatalysts.Using bismuth oxybromide(BiOBr)as a model system,we highlight that the light absorption cut-off edge could be effectively extended up to 500 nm by introducing Bi vacancies.On the basis of theoretical simulations and spectroscopic analyses,we attributed the broadening of light absorption to the promotion of excitonic transition that is generally forbidden in pristine BiOBr system,associated with Bi-vacancy-induced excited-state symmetry breaking.In addition,Bi vacancy was demonstrated to implement negligible effects on other photoexcitation properties like excited-state energy-level profiles and kinetics.Benefiting from these features,the defective sample exhibits a notable advantage in gaining visible-light-driven photocatalytic reactions.

关键词： semiconductor-based photocatalysts light absorption vacancy engineering excitonic transition selective oxidation

Genesis of ultra-deep dolostone and controlling factors of largescale reservoir:A case study of the Sinian Dengying Formation and the Cambrian Longwangmiao Formation in the Sichuan Basin

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Science China Earth Sciences 2024年第7期67卷 2352-2382页

作者： Xi LI Guangyou ZHU Zhiyao ZHANG PetroChina Research institute of Petroleum Exploration and Development Beijing 100083China School of Geosciences Yangtze UniversiyWuhan 430100China School of Earth Resoures China University of GeosciencesWuhan 430074China

This paper investigates the origin of ultra-deep dolostone and the factors influencing large-scale dolostone reservoirs,focusing on the Sinian Dengying Formation and the Cambrian Longwangmiao Formation in the Sichuan Basin.The study involves petrology,microscale X-ray diffraction,trace element analysis,and C-O-Sr-Mg isotope experiments to provide a detailed analysis.The research findings indicate that the Dengying and Longwangmiao formations comprise six types of matrix dolostone and four types of cement.The Dengying Formation,which developed under a sedimentary background of a restricted platform,contains special microbial and microcrystalline dolostones.The dolomite grains are small(30μm),high order degree(Min=0.7),small unit cell parameters,high Na content(Max=432 ppm),and low Fe and Mn content.The δ^(2

关键词： Ultra-deep layers Dolostone Supercontinent evolution microscale geochemistry Dengying Formation Longwangmiao Formation Sichuan Basin

Recent Advances in Strain-Induced Piezoelectric and Piezoresistive Effect-Engineered 2D Semiconductors for Adaptive Electronics and optoelectronics

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Nano-Micro Letters 2020年第8期12卷 236-279页

作者： Feng Li Tao Shen Cong Wang Yupeng Zhang Junjie Qi Han Zhang institute of microscale optoelectronics International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of EducationCollege of Physics and Optoelectronic EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China

The development of two-dimensional(2D)semiconductors has attracted widespread attentions in the scientific community and industry due to their ultra-thin thickness,unique structure,excellent optoelectronic properties and novel physics.The excellent flexibility and outstanding mechanical strength of 2D semiconductors provide opportunities for fabricated strain-sensitive devices and utilized strain tuning their electronic and optic–electric performance.The strain-engineered one-dimensional materials have been well investigated,while there is a long way to go for 2D semiconductors.In this review,starting with the fundamental theories of piezoelectric and piezoresistive effect resulted by strain,following we reviewed the recent simulation works of strain engineering in novel 2D semiconductors,such as Janus 2D and 2D-Xene structures.Moreover,recent advances in experimental observation of strain tuning PL spectra and transport behavior of 2D semiconductors are summarized.Furthermore,the applications of strain-engineered 2D semiconductors in sensors,photodetectors and nanogenerators are also highlighted.At last,we in-depth discussed future research directions of strain-engineered 2D semiconductor and related electronics and optoelectronics device applications.

关键词： 2D semiconductors Strain Piezoelectric effect Piezoresistive effect Electronic and optoelectronics

External field-strengthened Ostwald nanowelding

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Nano Research 2022年第5期15卷 4525-4535页

作者： Moxia Li Xi Xie Yaomengli Xu Jianfang Liu Yanan Fu Mei Han Xucheng Li Xidong Duan Changjun Min Jiawen Hu Hunan Key Laboratory of Two-Dimensional Materials Advanced Catalytic Engineering Research Center of the Ministry of Educationand College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China Nanophotonics Research Center Shenzhen Key Laboratory of Micro-Scale Optical Information Technology&Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China State Key Laboratory for Physical Chemistry of Solid Surfaces Xiamen UniversityXiamen 361005China

The accomplishment of nanowelding typically requires the input of high energy,possibly causing appreciable damages to the brittle nanomaterial.Herein,we report an external field(EF,i.e.,light,direct current(DC),and alternating current(AC))-strengthened Ostwald nanowelding(ONW)strategy to enable low-temperature nanowelding of Au nanoparticles(NPs)with nanoscale spacing in solution and propose an electron localization mechanism to understand it.We reveal that the EF-derived local electrons not only greatly strengthen the dissolution of surface atoms and the reduction of Au3+ions dissolved,but also confine(together with ordered water molecules)the transport of Au^(3+)ions within the nanogap.Consequently,the electrochemical Ostwald ripening(OR)process of the Au NPs is actively strengthened,which,along with the local electron-strengthened surface atom diffusion(as a result of the strong electrostatic repulsion created),enables feasible ONW for solution processing of interdigital electrodes(IDEs)from Au NPs and high-performance transparent conductor(TC)from Ag nanowires(NWs).Our low-temperature nanowelding strategy offers an efficient interconnection technique for the processing of functional nanodevices from individual nanomaterials.

关键词： external field(EF) Ostwald ripening(OR) nanowelding Au nanoparticle(NP) Ag nanowire(NWs)

Visible-light stimulated synaptic plasticity in amorphous indium−gallium−zinc oxide enabled by monocrystalline double perovskite for high-performance neuromorphic applications

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Nano Research 2023年第1期16卷 1304-1312页

作者： Fu Huang Feier Fang Yue Zheng Qi You Henan Li Shaofan Fang Xiangna Cong Ke Jiang Ye Wang Cheng Han Wei Chen Yumeng Shi International Collaborative Laboratory of 2D Materials for optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China College of Electronics and Information Engineering Shenzhen UniversityShenzhen 518060China Key Laboratory of Material Physics Ministry of EducationSchool of Physics and MicroelectronicsZhengzhou UniversityZhengzhou 450052China Department of Physics National University of SingaporeSingapore 117542Singapore Department of Chemistry National University of SingaporeSingapore 117543Singapore Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207China

Photoelectric synaptic devices have been considered as one of the key components in artificial neuromorphic systems due to their excellent capability to emulate the functions of visual neurons,such as light perception and image processing.Herein,we demonstrate an optically-stimulated artificial synapse with a clear photoresponse from ultraviolet to visible light,which is established on a novel heterostructure consisting of monocrystalline Cs2AgBiBr6 perovskite and indium–gallium–zinc oxide(IGZO)thin film.As compared with pure IGZO,the heterostructure significantly enhances the photoresponse and corresponding synaptic plasticity of the devices,which originate from the superior visible absorption of single-crystal Cs2AgBiBr6 and effective interfacial charge transfer from Cs2AgBiBr6 to IGZO.A variety of synaptic behaviors are realized on the fabricated thin-film transistors,including excitatory postsynaptic current,paired pulse facilitation,short-term,and long-term plasticity.Furthermore,an artificial neural network is simulated based on the photonic potentiation and electrical depression effects of synaptic devices,and an accuracy rate up to 83.8%±1.2%for pattern recognition is achieved.This finding promises a simple and efficient way to construct photoelectric synaptic devices with tunable spectrum for future neuromorphic applications.

关键词： artificial optoelectronic synapse monocrystalline Cs2AgBiBr6 thin-film transistors ultraviolet-to-visible neuromorphic computing

Syntheses and Crystal Structures of Two Novel Spiro Compounds Containing 1,5-Dioxaspiro[5.5]undecane-2,4-dione

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Chinese Journal of Structural Chemistry 2010年第5期29卷 696-699页

作者：曾伍兰孟庆国郭焕美张磊建方方 microscale Science institute Department of Chemistry and Chemical EngineeringWeifang University microscale Science institute Weifang University

Two novel spiro compounds,3-benzylidene-1,5-dioxaspiro[5.5]undecane-2,4-dione 1 and 3-（2-fluorobenzylidene）-1,5-dioxaspiro[5.5]undecane-2,4-dione 2,have been synthesized and characterized by X-ray single-crystal diffraction,IR and elemental analysis.Compound 1 belongs to the monoclinic system,space group P21/n with a=12.326（3）,b=5.6420（11）,c=20.089（4）,β= 101.79（3）o,C16H16O4,Mr= 272.29,V=1367.7（5）3,Z=4,Dc=1.322g/cm3,F（000）=576,μ（MoKa）=0.095 mm-1,the final R=0.0420 and wR=0.1159.Compound 2 is of monoclinic system,space group P21/n with a=12.283（3）,b=5.6367（11）,c=20.055（4）,β=102.00（3）o,C16H15FO4,Mr=290.28,V=1358.2（5）3,Z=4,Dc=1.420 g/cm3,F（000）=608,μ（MoKa）=0.110 mm-1,the final R=0.0353 and wR=0.0860.

关键词： synthesis crystal structure 1,5-dioxaspiro[5.5]undecane-2,4-dione spiro compounds