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Bifunctional noble-metal-free cocatalyst coating enabling better coupling of photocatalytic CO_(2)reduction and H_(2)O oxidation on direct Z-scheme heterojunction

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Nano research 2024年第6期17卷 5022-5030页

作者： Wei Zhao Weihao Mo Yan Zhang Lingxuan Hu Yiyi Zheng Zhulei Chen Xiangyue Niu Yuling Zhao Lichun Liu Shuxian Zhong Song Bai key laboratory of the Ministry of Education for advanced catalysis materials College of Chemistry and Materials ScienceZhejiang Normal UniversityJinhua 321004China College of Biological Chemical Sciences and Engineering and Nanotechnology Research InstituteJiaxing UniversityJiaxing 314001China College of Geography and Environmental Sciences Zhejiang Normal UniversityJinhua 321004China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China School of Biological and Chemical Engineering Panzhihua UniversityPanzhihua 617000China

Selective loading of spatially separated redox cocatalysts on direct Z-scheme heterojunctions holds great promise for advancing the efficiency of artificial photosynthesis,which however is limited to the photodeposition of noble metal cocatalysts and the fabrication of hollow double-shelled semiconductor heterojunctions.Moreover,the co-exposure of discrete cocatalyst and semiconductor increases the product diversity when both the exposed sites of which participate in CO_(2)photoreduction.Herein,we present a facile and versatile protocol to overcome these limitations via surface coating of Z-scheme heterojunctions with bifunctional noble-metal-free cocatalysts.With Cu_(2)O/Fe_(2)O_(3)(CF)as a model heterojunction and layered Ni(OH)_(2)as a model cocatalyst,it is found that Ni(OH)_(2)lying on the surfaces of Cu_(2)O and Fe_(2)O_(3)separately co-catalyzes the CO_(2)reduction and H_(2)O oxidation.Thorough experimental and theoretical investigation reveals that the Ni(OH)_(2)outer layer:(i)mitigates the charge recombination in CF and balances their transfer and consumption;(ii)reduces the rate-determining barriers for CO_(2)-to-CO and H_(2)O-to-O_(2)conversion,(iii)suppresses the side proton reduction occurring on CF,and(iv)protects the CF from component detachment.As expected,the redox reactions stoichiometrically proceed,and significantly enhanced photocatalytic activity,selectivity,and stability in CO generation are achieved by the stacked Cu_(2)O/Fe_(2)O_(3)@Ni(OH)_(2)in contrast to CF.This study demonstrates the significance of the synergy between bifunctional cocatalysts and Z-scheme heterojunctions for improving the efficacy of overall redox reactions,opening a fresh avenue for the rational design of artificial photosynthetic systems.

关键词： Z-scheme heterojunction bifunctional cocatalyst CO_(2)reduction H_(2)O oxidation stoichiometric redox reaction

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Asymmetrically coordinated main group atomic In-S_(1)N_(3)interface sites for promoting electrochemical CO_(2)reduction

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Nano research 2024年第6期17卷 5011-5021页

作者： Yan Gao Jinlong Ge Jingqiao Zhang Ting Cao Zhiyi Sun Wensheng Yan Yu Wang Jie Lin Wenxing Chen Zheng Liu Anhui Provincial Engineering laboratory of Silicon-based materials Bengbu UniversityBengbu 233030China State key laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China SEPA key laboratory of Eco-Industry Chinese Research Academy of Environmental SciencesBeijing 100012China Ningbo institute of materials Technology and Engineering Chinese Academy of ScienceNingbo 315201China Energy&catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China National Synchrotron Radiation laboratory University of Science and Technology of ChinaHefei 230029China Shanghai Synchrotron Radiation Facilities Shanghai Institute of Applied PhysicsChinese Academy of ScienceShanghai 201204China

Designing catalysts with highly active,selectivity,and stability for electrocatalytic CO_(2)to formate is currently a severe challenge.Herein,we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO_(2)reduction reaction.As expected,atomically dispersed In-based catalysts with In-S_(1)N_(3)atomic interface with asymmetrically coordinated exhibited high efficiency for CO_(2)reduction reaction(CO_(2)RR)to formate.It achieved a maximum Faradaic efficiency(FE)of 94.3%towards formate generation at−0.8 V vs.reversible hydrogen electrode(RHE),outperforming that of catalysts with In-S2N2 and In-N4 atomic interface.And at a potential of−1.10 V vs.RHE,In-S_(1)N_(3)achieves an impressive Faradaic efficiency of 93.7%in flow cell.The catalytic performance of In-S_(1)N_(3)sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure(XANES)measurements under electrochemical conditions.Our discovery provides the guidance for performance regulation of main group metal catalysts toward CO_(2)RR at atomic scale.

关键词： indium single-site catalyst main group metal asymmetrical coordination CO_(2)reduction reaction structure-activity relationship

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Simultaneously achieving high energy density and responsivity in submicron BaTiO_(3) film capacitors integrated on Si

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Journal of advanced Ceramics 2024年第2期13卷 198-206页

作者： Jun Ouyang Yinxiu Xue Chuanqi Song Meiling Yuan Kun Wang Yuyao Zhao Hongbo Cheng Hanfei Zhu Chao Liu institute of advanced Energy materials and Chemistry School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China key laboratory of key Film materials&Application for Equipment School of Material Sciences and EngineeringXiangtan UniversityXiangtan 411105China School of materials Science and Engineering Shandong UniversityJinan 250061China Academic Affairs Office Civil Aviation University of ChinaTianjin 300300China China Tobacco Shandong industrial Co. Ltd.Jinan 250014China

In the research field of energy storage dielectrics,the“responsivity”parameter,defined as the recyclable/recoverable energy density per unit electric field,has become critically important for a comprehensive evaluation of the energy storage capability of a dielectric.In this work,high recyclable energy density and responsivity,i.e.,W_(rec)=161.1 J·cm^(-3) and ξ=373.8 J·(kV·m^(2))^(-1),have been simultaneously achieved in a prototype perovskite dielectric,BaTiO_(3),which is integrated on Si at 500℃ in the form of a submicron thick film.This ferroelectric film features a multi-scale polar structure consisting of ferroelectric grains with different orientations and inner-grain ferroelastic domains.A LaNiO_(3) buffer layer is used to induce a{001}textured,columnar nanograin microstructure,while an elevated deposition temperature promotes lateral growth of the nanograins(in-plane diameter increases from~10-20 nm at lower temperatures to~30 nm).These preferably oriented and periodically regulated nanograins have resulted in a small remnant polarization and a delayed polarization saturation in the film’s P-E behavior,leading to a high recyclable energy density.Meanwhile,an improved polarizability/dielectric constant of the BaTiO_(3) film has produced a much larger maximum polarization than those deposited at lower temperatures at the same electric field,leading to a record-breaking responsivity for this simple perovskite.

关键词： energy storage energy density responsivity BaTiO_(3) dielectric capacitor Si

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Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries

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Chinese Chemical Letters 2024年第5期35卷 434-440页

作者： Haodong Wang Xiaoxu Lai Chi Chen Pei Shi Houzhao Wan Hao Wang Xingguang Chen Dan Sun CAS key laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial key laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and materials Fujian Normal UniversityFuzhou 350007China Xiamen institute of Rare Earth materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China School of Microelectronics Hubei UniversityWuhan 430062China Xiamen key laboratory of Rare Earth Photoelectric Functional materials Xiamen 361021China

The detrimental“shuttle effect”of lithium polysulfides(LiPSs)together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur(Li-S)batteries from commercial success.Here,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical performance.In this work,a two-dimensional(2D)rare-earth-based composite constructed by the layered gadolinium hydroxy chloride[Gd_(2)(OH)_(5)(H_(2)O)_(n)]Cl nanoplates(LGdH NPs)and graphene oxide(GO)was designed as a sulfur immobilizer for Li-S batteries.Combining the experimental results and density functional theory(DFT)calculations,it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling,but also acts as an effective catalyst to accelerate the liquid-solid conversion of polysulfides.The Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C,as well as excellent cycle stability with a decay rate of 0.087%over 500 cycles at 2 C.This study provided a deep understanding of the mechanism to suppress the“shuttle effect”by the LREHs,and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.

关键词： Lithium-sulfur batteries Functional separator Layered rare-earth hydroxides Shuttle effect Adsorption catalysis

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Two-dimensional materials for future information technology: status and prospects

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Science China(Information Sciences) 2024年第6期67卷 1-147页

作者： Hao QIU Zhihao YU Tiange ZHAO Qi ZHANG Mingsheng XU Peifeng LI Taotao LI Wenzhong BAO Yang CHAI Shula CHEN Yiqi CHEN Hui-Ming CHENG Daoxin DAI Zengfeng DI Zhuo DONG Xidong DUAN Yuhan FENG Yu FU Jingshu GUO Pengwen GUO Yue HAO Jun HE Xiao HE Jingyi HU Weida HU Zehua HU Xinyue HUANG Ziyang HUANG Ali IMRAN Ziqiang KONG Jia LI Qian LI Weisheng LI Lei LIAO Bilu LIU Can LIU Chunsen LIU Guanyu LIU Kaihui LIU Liwei LIU Sheng LIU Yuan LIU Donglin LU Likuan MA Feng MIAO Zhenhua NI Jing NING Anlian PAN Tian-Ling REN Haowen SHU Litao SUN Yue SUN Quanyang TAO Zi-Ao TIAN Dong WANG Hao WANG Haomin WANG Jialong WANG Junyong WANG Wenhui WANG Xingjun WANG Yeliang WANG Yuwei WANG Zhenyu WANG Yao WE Department of Applied Physics The Hong Kong Polytechnic University key laboratory for Micro-Nano Physics and Technology of Hunan Province College of Materials Science and EngineeringHunan University College of Integrated Circuits Zhejiang University Shenzhen Geim Graphene Center Shenzhen Key Laboratory of Layered Materials for Value-Added ApplicationsTsinghua-Berkeley Shenzhen Institute & Institute of Materials ResearchTsinghua Shenzhen International Graduate SchoolTsinghua University State key laboratory of Extreme Photonics and Instrumentation College of Optical Science and EngineeringInternational Research Center for Advanced PhotonicsZijingang CampusZhejiang University National key laboratory of materials for Integrated Circuits Shanghai Institute of Microsystem and Information TechnologyChinese Academy of Sciences CAS key laboratory of Nanophotonic materials and Devices & key laboratory of Nanodevices and Applications i-LabSuzhou Institute of Nano-Tech and Nano-Bionics (SINANO)Chinese Academy of Sciences College of Chemistry and Chemical Engineering Hunan University key laboratory of Quantum State Construction and Manipulation (Ministry of Education) Department of PhysicsRenmin University of China School of Integrated Circuits Beijing National Research Center for Information Science and Technology (BNRist)Tsinghua University School of Electronic Science and Engineering Nanjing University The State key Discipline laboratory of Wide Band Gap Semiconductor Technology Shaanxi Joint Key Laboratory of GrapheneSchool of MicroelectronicsXidian University key laboratory of Artificial Micro- and Nano-Structures of Ministry of Education School of Physics and TechnologyWuhan University School of Integrated Circuits Huazhong University of Science and Technology Center for Nanochemistry (CNC) Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking University State key laboratory for Artificial Microstruct

Over the past 70 years, the semiconductor industry has undergone transformative changes,largely driven by the miniaturization of devices and the integration of innovative structures and materials. Two-dimensional(2D) materials like transition metal dichalcogenides(TMDs) and graphene are pivotal in overcoming the limitations of silicon-based technologies, offering innovative approaches in transistor design and functionality, enabling atomic-thin channel transistors and monolithic 3D integration. We review the important progress in the application of 2D materials in future information technology, focusing in particular on microelectronics and optoelectronics. We comprehensively summarize the key advancements across material production, characterization metrology, electronic devices, optoelectronic devices, and heterogeneous integration on silicon. A strategic roadmap and key challenges for the transition of 2D materials from basic research to industrial development are outlined. To facilitate such a transition, key technologies and tools dedicated to 2D materials must be developed to meet industrial standards, and the employment of AI in material growth, characterizations, and circuit design will be essential. It is time for academia to actively engage with industry to drive the next 10 years of 2D material research.

关键词： two-dimensional (2D) materials information technology production technology standardization of characterization microelectronicdevices optoelectronic devices multi-functional integration

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Protein-activated atomic layer deposition for robust crude-oil-repellent hierarchical nano-armored membranes

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Science Bulletin 2024年第2期69卷 218-226页

作者： Xiaobin Yang Pan Sun Yajie Wen Anil U.Mane Jeffrey W.Elam Jun Ma Shaomin Liu Seth B.Darling Lu Shao MIIT key laboratory of Critical materials Technology for New Energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China Chemical Sciences and Engineering Division Argonne National LaboratoryLemont IL 60439USA Applied materials Division Argonne National LaboratoryLemont IL 60439USA advanced materials for Energy-Water Systems Energy Frontier research Center Argonne National LaboratoryLemont IL 60439USA Pritzker School of Molecular Engineering University of ChicagoChicago IL 60637USA Department of Physics University of Ilinois at ChicagoChicago IL 60607USA School of Environment Harbin Institute of TechnologyHarbin 150090China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerth WA 6845Australia

Atomic layer deposition(ALD)offers unique capabilities to fabricate atomically engineered porous materials with precise pore tuning and multi-functionalization for diverse applications like advanced membrane separations towards sustainable energy-water systems.However,current ALD technique is inhibited on most non-polar polymeric membranes due to lack of accessible nucleation sites.Here,we report a facile method to efficiently promote ALD coating on hydrophobic surface of polymeric membranes via novel protein activation/sensitization.As a proof of concept,TiO2 ALD-coated membranes activated by bovine serum albumin exhibit remarkable superhydrophilicity,ultralow underwater crude oil adhesion,and robust tolerance to rigorous environments including acid,alkali,saline,and ethanol.Most importantly,excellent cyclable crude oil-in-water emulsion separation performance can be achieved.The mechanism for activation/sensitization is rooted in reactivity for a particular set of amino acids.Furthermore,the universality of protein-sensitized ALD is demonstrated using common egg white,promising numerous potential usages in biomedical engineering,environmental remediation,lowcarbon manufacturing,catalysis,and beyond.

关键词： Membrane separation Atomic layer deposition Water treatment Antifouling

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Insights into ionic association boosting water oxidation activity and dynamic stability

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Journal of Energy Chemistry 2024年第2期89卷 99-109,I0004页

作者： Zanling Huang Shuqi Zhu Yuan Duan Chaoran Pi Xuming Zhang Abebe Reda Woldu Jing-Xin Jian Paul K.Chu Qing-Xiao Tong Liangsheng Hu Xiangdong Yao Department of Chemistry and key laboratory for Preparation and Application of Ordered Structural materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina Chemistry and Chemical Engineering Guangdong laboratory Shantou 515063GuangdongChina State key laboratory of Refractories and Metallurgy and institute of advanced materials and Nanotechnology Wuhan University of Science and TechnologyWuhan 430081HubeiChina Department of Physics Department of Materials Science and Engineeringand Department of Biomedical EngineeringCity University of Hong KongTat Chee AvenueKowloonHong KongChina School of advanced Energy Sun Yat-sen University(Shenzhen)Shenzhen 518107GuangdongChina

There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.

关键词： Oxygen evolution reaction Fe(Ⅲ)-catalysis Ni-Fe binary active centers Ion-catalyzed effects Robust stability

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Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts

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Transactions of Tianjin University 2024年第1期30卷 90-102页

作者： Xincheng Li Yunhao Liu Dejian Zhao Shuaishuai Lyu Jingwei Ye Xiaoshen Li Peipei Wu Ye Tian Yingtian Zhang Tong Ding Song Song Qingpeng Cheng Xingang Li State key laboratory of Chemical Engineering Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Haihe Laboratory of Sustainable Chemical TransformationsTianjin Key Laboratory of Applied Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang institute of Tianjin University Shaoxing 312300China Sinopec research institute of Petroleum Processing Co. LTDBeijing 100083China Physical Sciences and Engineering Division Advanced Membranes and Porous Materials(AMPM)CenterKing Abdullah University of Science and Technology(KAUST)23955-6900 ThuwalSaudi Arabia

Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.

关键词： Fischer-Tropsch synthesis N-doped carbon materials Ruthenium catalyst Pyridinic N Metal-N interaction

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Non-bonding modulations between single atomic cerium and monodispersed selenium sites towards efficient oxygen reduction

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Nano research 2024年第6期17卷 4753-4763页

作者： Leilei Yin Shuai Zhang Mingzi Sun Siyuan Wang Bolong Huang Yaping Du Tianjin key Lab for Rare Earth materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina research Centre for Carbon-Strategic catalysis The Hong Kong Polytechnic UniversityHung HomKowloon 999077Hong KongChina

Currently,dual atomic catalysts(DACs)with neighboring active sites for oxygen reduction reaction(ORR)still meet lots of challenges in the synthesis,especially the construction of atomic pairs of elements from different blocks of the periodic table.Herein,a“rare earth(Ce)-metalloid(Se)”non-bonding heteronuclear diatomic electrocatalyst has been constructed for ORR by rational coordination and carbon support defect engineering.Encouraging,the optimized Ce-Se diatomic catalysts(Ce-Se DAs/NC)displayed a half-wave potential of 0.886 V vs.reversible hydrogen electrode(RHE)and excellent stability,which surpass those of separate Ce or Se single atoms and most single/dual atomic catalysts ever reported.In addition,a primary zinc-air battery constructed using Ce-Se DAs/NC delivers a higher peak power density(209.2 mW·cm^(−2))and specific capacity(786.4 mAh·gZn^(−1))than state-of-the-art noble metal catalysts Pt/C.Theoretical calculations reveal that the Ce-Se DAs/NC has improved the electroactivity of the Ce-N_(4)region due to the electron transfer towards the nearby Se specific activity(SA)sites.Meanwhile,the more electron-rich Se sites promote the adsorptions of key intermediates,which results in the optimal performances of ORR on Ce-Se DAs/NC.This work provides new perspectives on electronic structure modulations via non-bonded long-range coordination micro-environment engineering in DACs for efficient electrocatalysis.

关键词： catalyst rare earth oxygen reduction reaction(ORR) metalloid non-bonding modulation

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Effect of coil and chamber structure on plasma radial uniformity in radio frequency inductively coupled plasma

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Plasma Science and Technology 2024年第7期26卷 58-66页

作者：赵洋周晓华高升荣宋莎莎赵玉真 Shaanxi International Joint research Center for Applied Technology of Controllable Neutron Source Xijing UniversityXi’an 710123People’s Republic of China Technological institute of materials&Energy Science(TIMES) Xi’an Key Laboratory of Advanced Photo-electronics Materials and Energy Conversion DeviceSchool of Electronic InformationXijing UniversityXi’an 710123People’s Republic of China

Enhancing plasma uniformity can be achieved by modifying coil and chamber structures in radio frequency inductively coupled plasma(ICP)to meet the demand for large-area and uniformly distributed plasma in industrial manufacturing.This study utilized a two-dimensional self-consistent fluid model to investigate how different coil configurations and chamber aspect ratios affect the radial uniformity of plasma in radio frequency ICP.The findings indicate that optimizing the radial spacing of the coil enhances plasma uniformity but with a reduction in electron density.Furthermore,optimizing the coil within the ICP reactor,using the interior point method in the Interior Point Optimizer significantly enhances plasma uniformity,elevating it from 56%to 96%within the range of the model sizes.Additionally,when the chamber aspect ratio k changes from 2.8 to 4.7,the plasma distribution changes from a center-high to a saddleshaped distribution.Moreover,the plasma uniformity becomes worse.Finally,adjusting process parameters,such as increasing source power and gas pressure,can enhance plasma uniformity.These findings contribute to optimizing the etching process by improving plasma radial uniformity.

关键词： inductively coupled plasma fluid simulation optimized coil chamber aspect ratio plasma uniformity

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