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Recent progress on surface chemistryⅠ:Assembly and reaction

Chinese chemical Letters 2024年第12期35卷 43-94页

作者： Xin Li Zhen Xu Donglei Bu Jinming Cai Huamei Chen Qi Chen Ting Chen Fang Cheng Lifeng Chi Wenjie Dong Zhenchao Dong Shixuan Du Qitang Fan Xing Fan Qiang Fu Song Gao Jing Guo Weijun Guo Yang He Shimin Hou Ying Jiang Huihui Kong Baojun Li Dengyuan Li Jie Li Qing Li Ruoning Li Shuying Li Yuxuan Lin Mengxi Liu Peinian Liu Yanyan Liu Jingtao Lü Chuanxu Ma Haoyang Pan JinLiang Pan Minghu Pan Xiaohui Qiu Ziyong Shen Shijing Tan Bing Wang Dong Wang Li Wang Lili Wang Tao Wang Xiang Wang Xingyue Wang Xueyan Wang Yansong Wang Yu Wang Kai Wu Wei Xu Na Xue Linghao Yan Fan Yang Zhiyong Yang Chi Zhang Xue Zhang Yang Zhang Yao Zhang Xiong Zhou Junfa Zhu Yajie Zhang Feixue Gao Yongfeng Wang Center for Carbon-based Electronics and Key Laboratory for the Physics and Chemistry of Nanodevices School of ElectronicsPeking UniversityBeijing 100871China Spin-X Institute School of MicroelectronicsSouth China University of TechnologyGuangzhou 511442China School of Materials and Energy Guangzhou Key Laboratory of Low-Dimensional Materials and Energy Storage DevicesGuangdong University of TechnologyGuangzhou 510006China Faculty of Materials Science and Engineering Kunming University of Science and TechnologyKunming 650093 China i-Lab CAS Key Laboratory of Nanophotonic Materials and DevicesSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of SciencesBeijing 100190China State Key Laboratory for Organic Electronics and Information Displays&Jiangsu Key Laboratory for Biosensors Institute of Advanced MaterialsJiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing University of Posts and TelecommunicationsNanjing 210023China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics University of Science and Technology of ChinaHefei 230026China Institute of Physics&University of Chinese Academy of Sciences Beijing 100190China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Chemistry Beijing Normal UniversityBeijing 100875China Beijing National Laboratory for Molecular Sciences(BNLMS) College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China School

Surface chemistry focuses on the investigation of the adsorption,migration,assembly,activation,reaction,and desorption of atoms and molecules at *** chemistry plays the pivotal roles in both fundamental science and applied *** review will summarize the recent progresses on surface assembly,synthesis and catalysis investigated mainly by scanning tunneling microscopy and atomic force *** assemblies of water and small biomolecules,construction of Sierpin′ski triangles and surface chirality are ***-surface synthesis of conjugated carbo-and heterocycles and other kinds of carbon nanostructures are *** model catalysis,including single-atom catalysis and electrochemical catalysis,are discussed at the single-atom level.

关键词： Surface chemistry Assembly Surface synthesis Catalysis on surface Surface electrochemical processes

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Alkyl-thiophene-alkyl linkers to construct double-cable conjugated polymers for single-component organic solar cells

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Chinese chemical Letters 2024年第1期35卷 542-546页

作者： Wenbin Lai Safakath Karuthedath Chengyi Xiao Lei Meng Frédéric Laquai Weiwei Li Yongfang Li Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Beijing Advanced Innovation Center for Soft Matter Science and Engineering&State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China King Abdullah University of Science and Technology(KAUST) KAUST Solar Center(KSC)Physical Sciences and Engineering Division(PSE)Material Science and Engineering Program(MSE)Thuwal 23955-6900Kingdom of Saudi Arabia University of Chinese Academy of Sciences Beijing 100049China Institute of Materials Research Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

In this work,semirigid linkers of the alkyl-thiophene-alkyl structure are developed to construct double-cable *** alkyl units,propyl(C3H6),hexyl(C6H12),and dodecyl(C12H24),are applied as semirigid linkers,yielding three double-cable polymers:PBC6-T,PBC12-T,and PBC24-T,***12-T which uses C6H12-thiophene-C6H12 linkers is found to exhibit the best device efficiency of 5.56%,while PBC6-T and PBC24-T with shorter or longer linkers yield device efficiencies of only 2.65%and 1.09%in single-component organic solar cells(SCOSCs).Further studies reveal that PBC12-T exhibits higher crystallinity and improved charge transport,resulting in better *** work provides an approach to construct double-cable conjugated polymers with long alkyl linkers,and it shows the importance of the linker length for the photovoltaic performance of SCOSCs.

关键词： Double-cable conjugated polymer Single-component organic solar cell Crystallinity Semirigid linkers Alkyl-thiophene-alkyl

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Titania-Morphology-Dependent Pt-TiO₂ Interfacial Catalysis in Water-Gas Shift Reaction

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ACS Catalysis 2023年第1期13卷 392-399页

作者： Zhang, Yunshang Jia, Aiping Li, Zhaorui Yuan, Zhenxuan Huang, Weixin Hefei National Research Center for Physical Sciences at the Microscale iChEM Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes Department of Chemical Physics University of Science and Technology of China Hefei 230026 China Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical Chemistry Zhejiang Normal University Jinhua 321004 China

The bifunctional role of the noble-metal-oxide interface in activating reactants is important for efficient heterogeneous catalysis of the water-gas shift (WGS) reaction. Herein, we report that the morphology of the TiO₂ support strongly affects the Pt-TiO₂ interfacial catalysis for the WGS reaction using Pt nanoparticles of similar sizes supported on anatase TiO₂ nanocrystals with various morphologies predominantly exposing {001} facets (denoted TiO₂{001}), {100} facets (denoted TiO₂{100}), and {101} facets (denoted TiO₂{101}). CO conversions follow the order Pt/TiO₂{100} ≈ Pt/TiO₂{101} > Pt/TiO₂{001}, but the apparent activation energies are similar for Pt/TiO₂{100}, Pt/TiO₂{101}, and Pt/TiO₂{001} catalysts. Characterization results show that the Pt/TiO₂{001} catalyst exhibits fewer surface oxygen vacancies and consequently active Pt-O_v,TiO interfacial ensemble sites than Pt/TiO₂{100} and Pt/TiO₂{101} catalysts. This can be attributed to the fact that oxygen vacancies are more stable in the bulk of TiO₂{001} than on the surface but are more stable on the surface of TiO₂{100} and TiO₂{101} than in the bulk and to the fact that carbonate and bicarbonate spectators accumulate at the Pt-TiO₂ interface at the Pt/TiO₂{001} catalyst but barely accumulate the at Pt/TiO₂{100} and Pt/TiO₂{101} catalysts. Both lead to the poorer catalytic activity of Pt/TiO₂{001} catalyst for catalyzing the WGS reaction. These results provide insights into a fundamental understanding of the activity-structure relation of Pt/TiO₂ catalysts for the WGS reaction. © 2022 American chemical Society

关键词： facet effects interfacial catalysis metal−support interaction Pt/TiO2 structure−activity relation

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Semitransparent organic photovoltaics enabled by transparent p-type inorganic semiconductor and near-infrared acceptor

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Journal of Energy Chemistry 2024年第9期96卷 351-358页

作者： Xue Yan Jiayu Wang Wei He Top Archie Dela Peña Can Zhu Hailin Yu Yingyue Hu Cenqi Yan Shengqiang Ren Xingyu Chen Zhe Wang Jiaying Wu Mingjie Li Jianlong Xia Lei Meng Shirong Lu Dewei Zhao Mikhail Artemyev Yongfang Li Pei Cheng College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina Department of Applied Physics The Hong Kong Polytechnic UniversityKowloonHong Kong 999077China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China College of Materials Science and Engineering&Engineering Research Center of Alternative Energy Materials&Devices Ministry of EducationSichuan UniversityChengdu 610065SichuanChina Department of Material Science and Technology Taizhou UniversityTaizhou 318000ZhejiangChina Advanced Materials Thrust Function HubThe Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400GuangdongChina State Key Laboratory of Advanced Technology for Materials Science and Processing Center of Smart Materials and DevicesWuhan University of TechnologyWuhan 430070HubeiChina Department of Civil1nd Environmental Engineering The Hong Kong University of Science and TechnologyHong Kong 999077China Research Institute for Physical Chemical Problems Belarusian State UniversityMinsk 220006Belarus

Semitransparent organic photovoltaics(STOPVs)have gained wide attention owing to their promising applications in building-integrated photovoltaics,agrivoltaics,and floating *** semiconductors with high charge carrier mobility usually have planar and conjugated structures,thereby showing strong absorption in visible *** this work,a new concept of incorporating transparent inorganic semiconductors is proposed for high-performance ***(I)thiocyanate(CuSCN)is a visible-transparent inorganic semiconductor with an ionization potential of 5.45 eV and high hole *** transparency of CuSCN benefits high average visible transmittance(AVT)of *** energy levels of CuSCN as donor match those of near-infrared small molecule acceptor BTP-eC9,and the formed heterojunction exhibits an ability of exciton *** mobility of CuSCN contributes to a more favorable charge transport channel and suppresses charge *** control STOPVs based on PM6/BTP-eC9 exhibit an AVT of 19.0%with a power conversion efficiency(PCE)of 12.7%.Partial replacement of PM6 with CuSCN leads to a 63%increase in transmittance,resulting in a higher AVT of 30.9%and a comparable PCE of 10.8%.

关键词： Copper(I)thiocyanate Inorganic semiconductor Semitransparent Organic photovoltaics Charge dissociation

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JARVIS-Leaderboard:a large scale benchmark of materials design methods

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npj Computational Materials 2024年第1期10卷 2280-2296页

作者： Kamal Choudhary Daniel Wines Kangming Li Kevin F.Garrity Vishu Gupta Aldo H.Romero Jaron T.Krogel Kayahan Saritas Addis Fuhr Panchapakesan Ganesh Paul R.C.Kent Keqiang Yan Yuchao Lin Shuiwang Ji Ben Blaiszik Patrick Reiser Pascal Friederich Ankit Agrawal Pratyush Tiwary Eric Beyerle Peter Minch Trevor David Rhone Ichiro Takeuchi Robert B.Wexler Arun Mannodi-Kanakkithodi Elif Ertekin Avanish Mishra Nithin Mathew Mitchell Wood Andrew Dale Rohskopf Jason Hattrick-Simpers Shih-Han Wang Luke E.K.Achenie Hongliang Xin Maureen Williams Adam J.Biacchi Francesca Tavazza Material Measurement Laboratory National Institute of Standards and TechnologyGaithersburgMD20899USA Department of Materials Science and Engineering University of Toronto27 King’s College CirTorontoONCanada Department of Electrical and Computer Engineering Northwestern UniversityEvanstonIL 60208USA Lewis-Sigler Institute for Integrative Genomics Princeton UniversityPrincetonNJ 08544USA Ludwig Institute for Cancer Research Princeton UniversityPrincetonNJ 08544USA Department of Physics and Astronomy West Virginia UniversityMorgantownWV 26506USA Materials Science and Technology Division Oak Ridge National LaboratoryOak RidgeTN 37831USA Center for Nanophase Materials Science Oak Ridge National LaboratoryOak RidgeTN 37831USA Computational Sciences and Engineering Division Oak Ridge National LaboratoryOak RidgeTN 37831USA Department of Computer Science and Engineering Texas A&M UniversityCollege StationTX 77843USA Globus University of ChicagoChicagoIL 60637USA Data Science and Learning Division Argonne National LabLemontIL 60439USA Institute of Nanotechnology Karlsruhe Institute of TechnologyKaiserstraße 1276131 KarlsruheGermany Institute of Theoretical Informatics Karlsruhe Institute of TechnologyKaiserstraße 1276131 KarlsruheGermany Department of Chemistry and Biochemistry and Institute for Physical Science and Technology University of MarylandCollege ParkMD 20742USA Department of Physics Applied Physics and AstronomyRensselaer Polytechnic InstituteTroyNY12180USA Department of Materials Science and Engineering University of MarylandCollege ParkMD20742USA Department of Chemistry and Institute of Materials Science and Engineering Washington University in St.LouisSt.LouisMO63130USA School of Materials Engineering Purdue UniversityWest LafayetteIN47907USA Department of Mechanical Science and Engineering University of Illinois Urbana-ChampaignUrbanaIllinois 61801USA Materials Research Laboratory University of Illinois Urbana-ChampaignUrbanaIL 61801USA Theore

Lack of rigorous reproducibility and validation are significant hurdles for scientific development across many *** science,in particular,encompasses a variety of experimental and theoretical approaches that require careful *** efforts have been developed previously to mitigate these ***,a comprehensive comparison and benchmarking on an integrated platform with multiple data modalities with perfect and defect materials data is still *** work introduces JARVIS-Leaderboard,an open-source and community-driven platform that facilitates benchmarking and enhances *** platform allows users to set up benchmarks with customtasks and enables contributions in the form of dataset,code,and meta-data *** cover the following materials design categories:Artificial Intelligence(AI),Electronic Structure(ES).

关键词： rigorous perfect enable

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Electrostatically responsive liquid gating system for controlled microbubble generation

Industrial Chemistry & Materials

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Industrial Chemistry & Materials 2024年第3期2卷 424-431页

作者： Guochao Zeng Yunmao Zhang Zhongyi Fang Lejian Yu Yawen Zhang Shaojie Wang Xu Hou State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchJiujiang Research InstituteCollege of Physical Science and TechnologyXiamen UniversityXiamen 361005China Department of Joint Surgery and Sports Medicine Zhongshan HospitalXiamen UniversityXiamen 361004China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Microbubbles have attracted considerable attention due to their distinctive properties,such as large surface area,inherent selfcompression,and exceptional mass transfer *** features render microbubbles valuable across a diverse range of industries,such as water treatment,mineral flotation,and the food *** several methods for microbubble generation exist,the gas–liquid membrane dispersion technique emerges as a reproducible and efficient ***,conventional approaches struggle to achieve active in situ control of bubble *** this study,we introduce an electrostatically responsive liquid gating system(ERLGS)designed for the active management of microbubble *** electric fields and anionic surfactants,our system showcases the capability to dynamically regulate bubble size by manipulating the solid–liquid *** confirm that this active control relies on the electrostatic adsorption and desorption of anionic surfactants,thereby regulating the interactions among the solid–liquid–gas *** research elucidates the ERLGS's ability of precisely controlling the generation of bubbles in situ,enabling nearly one-order-of-magnitude change in bubble size,underscoring its applicability in various fields.

关键词： Liquid gating system Electrostatic response Anionic surfactants Adsorption and desorption Microbubbles

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Jahn-Teller Effect Directed Bandgap Tuning of Birnessite for Pseudocapacitive Application

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Energy & Environmental Materials 2023年第3期6卷 222-228页

作者： Sheng Zhu Yuechao Wang Jinshu Zhang Jian Sheng Feng Yang Meng Wang Jiangfeng Ni Hong Jiang Yan Li Beijing National Laboratory for Molecular Sciences Key Laboratory for the Physics and Chemistry of NanodevicesState Key Laboratory of Rare Earth Materials Chemistry and ApplicationsCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Institute of Molecular Science Key Laboratory of Chemical Biology and Molecular Engineering of Education MinistryShanxi UniversityTaiyuan 030006China Beijing National Laboratory for Molecular Sciences Institute of Theoretical and Computational ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China School of Physical Science and Technology Center for Energy Conversion Materials&Physics(CECMP)Jiangsu Key Laboratory of Thin FilmsSoochow UniversitySuzhou 215006China

Birnessite M_(x)MnO_(2)(M=Na^(+),K^(+),etc.)has emerged as a promising alternative to the classical MnO_(2)material owing to its improved pseudocapacitive performance for energy *** their structure–property correlation is essential for the development and application of advanced ***,we adopt the crystal field theory and density functional simulation to reveal the structural dependence of the pseudocapacitive property of M_(x)MnO_(2).Attributing to the Jahn–Teller effect of Mn^(3+),the bandgap of Kx MnO_(2)can be tuned by changing the x value(i.e.,the Mn(III)/Mn(IV)ratio).Then,we design a narrow-bandgap K 0.25 MnO_(2)(0.84 eV),which affords a high capacitance of 415 F g^(-1)at 1 A g^(-1)and a desirable rate capability of 293 F g^(-1)at 20 A g^(-1).Operando Raman spectroscopy confirms that the Jahn–Teller induced structure evolution of[MnO_(6)]octahedron accounts for the superior pseudocapacitive behavior of K_(0.25)MnO_(2).This finding offers theoretical guidance to the design and application of birnessite materials for pseudocapacitors.

关键词： birnessite charge storage Jahn–Teller effect manganese dioxide supercapacitor

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Doppler-free spectroscopy of an atomic beam probed in traveling-wave fields

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physical Review A 2023年第4期107卷 042811-042811页

作者： Jin-Lu Wen (温金录) Jia-Dong Tang (唐家栋) Jun-Feng Dong (董俊峰) Xiao-Jiao Du (杜小娇) Shui-Ming Hu (胡水明) Y. R. Sun (孙羽) Department of Chemical Physics University of Science and Technology of China Hefei 230026 China Hefei National Research Center of Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 China Institute of Advanced Science Facilities Shenzhen 518107 China

We propose a method to probe the precision spectroscopy of an atomic beam using traveling-wave laser beams. The method is demonstrated by measuring the 23S−23P transition in a slow helium atomic beam. The first-order Doppler shift could be effectively suppressed by up to three orders of magnitude compared to that induced by the probing light beam. This method avoids using a standing-wave field when probing the spectra, and consequently, it reduces the laser power dependence and eliminates the modulation due to the standing-wave field. Preliminary measurements of the 23S−23P transition of He4 indicate that the uncertainty could be reduced to the sub-kHz level.

关键词： Atomic spectra

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Polarizability of molecular hydrogen and gas metrology

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physical Review A 2025年第1期111卷 012801-012801页

作者： Zhong-Liang Nie (聂中梁) Jin Wang (王进) Chang-Le Hu (胡常乐) Yu R. Sun (孙羽) Cun-Feng Cheng (程存峰) Yan Tan (谈艳) Shui-Ming Hu (胡水明) Hefei National Research Center of Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 China Hefei National Laboratory University of Science and Technology of China Hefei 230088 China State Key Laboratory of Molecular Reaction Dynamics Department of Chemical Physics University of Science and Technology of China Hefei 230026 China Institute of Advanced Science Facilities Shenzhen 518107 China

The polarizability of the hydrogen molecule can be precisely calculated based on the quantum electrodynamics (QED) theory and a few fundamental physical constants. Therefore, experimental measurements with comparable accuracy can test the theory and establish gas metrology with hydrogen as the working gas. An optical refractometer was built and its performance was tested by measuring the electric dipole polarizabilities of argon, neon, and nitrogen. The polarizability of the H2 molecule was determined to be 2.031 027(71) cm3mol−1. The result agrees with the current calculated value, indicating the potential of a primary standard for pressure or temperature through measuring the polarizability of H2.

关键词： Molecules

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原位重构限制在三维纳米孔铜内的铋纳米颗粒促电还原CO_(2)

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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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