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Electron-deficient ZnO induced by heterointerface engineering as the dominant active component to boost CO_(2)-to-formate conversion

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Carbon Energy 2024年第5期6卷 127-136页

作者： Qing Qin Zijian Li Yingzheng Zhang Haeseong Jang Li Zhai Liqiang Hou Xiaoqian Wei Zhe Wang Min Gyu Kim Shangguo Liu Xien Liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdaoChina Department of Chemistry City University of Hong KongHong Kong SARChina Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-doRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)PohangRepublic of Korea

Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.

关键词： charge redistribution CO_(2)reduction reaction electrocatalyst heterointerfaces selectivity

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Co_(3)O_(4)/Mn_(3)O_(4) hybrid catalysts with heterointerfaces as bifunctional catalysts for Zn-air batteries

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Journal of Energy Chemistry 2022年第5期31卷 679-687页

作者： Qikai Huang Xiongwei Zhong Qi Zhang Xin Wu Miaolun Jiao Biao Chen Jinzhi Sheng Guangmin Zhou Shenzhen Geim Graphene Center Tsinghua-Berkeley Shenzhen Institute&Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055GuangdongChina

Zinc-air batteries(ZABs) with high energy density and safety are promising as next-generation energy storage systems, while their applications are severely hindered by the sluggish reaction kinetic of air cathodes. Developing a bifunctional catalyst with high activity and durability is an effective strategy to address the above challenges. Herein, a Co_(3)O_(4)/Mn_(3)O_(4) nanohybrid with heterointerfaces is designed as advanced cathode catalyst for ZABs. Density functional theory calculations show the heterogeneous interface between Co_(3)O_(4)/Mn_(3)O_(4) can improve the dynamics of carrier transport and thus enhancing the catalytic activity and durability. The Co_(3)O_(4)/Mn_(3)O_(4) catalyst anchored on reduced graphene oxide(rGO)exhibits high oxygen reduction reaction(ORR) activity with a half-wave potential of 0.86 V, and excellent oxygen evolution reaction(OER) activity with the potential of 1.59 V at 10 mA cm^(-2) , which are comparable to the commercial noble metal catalysts. The improved ORR/OER catalytic activity is ascribed to the synergistic effect of heterointerfaces between Co_(3)O_(4) and Mn_(3)O_(4)as well as the improved conductivity and contact area of oxygen/catalysts/electrolytes three-phase interface by r GO. Furthermore, a home-made ZAB based on Co_(3)O_(4)/Mn_(3)O_(4)/r GO shows a high open circuit voltage of 1.54 V, a large power density of 194.6 mW cm^(-2) and good long-term cycling stability of nearly 400 h at 5 mA cm^(-2) , which affords a promising bifunctional oxygen catalyst for rechargeable ZABs.

关键词： Transition metal oxide Carbon-based catalyst heterointerfaces Bifunctional catalyst Zn-air batteries

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In-situ electrochemical restructuring of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces enabling stabilization intermediates for high-performance CO_(2)electroreduction to formate

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Nano Research 2023年第5期16卷 7974-7981页

作者： Xiaofeng Yang Qinru Wang Feiran Chen Hu Zang Changjiang Liu Nan Yu Baoyou Geng College of Chemistry and Materials Science the Key Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesAnhui Provincial Engineering Laboratory for New-Energy Vehicle Battery Energy-Storage MaterialsAnhui Normal UniversityWuhu 241002China Institute of Energy Hefei Comprehensive National Science CenterHefei 230031China

Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.

关键词： in-situ electrochemical restructuring heterointerfaces CO_(2)electroreduction formate current density

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Nanoscale All-Oxide-Heterostructured Bio-inspired Optoresponsive Nociceptor

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Nano-Micro Letters 2020年第7期12卷 13-28页

作者： Mohammad Karbalaei Akbari Jie Hu Francis Verpoort Hongliang Lu Serge Zhuiykov Centre for Environmental and Energy Research Ghent University Global CampusIncheonSouth Korea Department of Green Chemistry and Technology Faculty of Bioscience EngineeringGhent University9000 GhentBelgium College of Information Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiPeople’s Republic of China Laboratory of Organometallics Catalysis and Ordered MaterialsState Key Laboratory of Advanced Technology for Materials Synthesis and ProcessingWuhan University of TechnologyWuhan 430070People’s Republic of China School of Microelectronic Fudan UniversityShanghai 200433People’s Republic of China

Retina nociceptor,as a key sensory receptor,not only enables the transport of warning signals to the human central nervous system upon its exposure to noxious stimuli,but also triggers the motor response that minimizes potential sensitization.In this study,the capability of two-dimensional all-oxide-heterostructured artificial nociceptor as a single device with tunable properties was confirmed.Newly designed nociceptors utilize ultra-thin sub-stoichiometric TiO2–Ga2O3 heterostructures,where the thermally annealed Ga2O3 films play the role of charge transfer controlling component.It is discovered that the phase transformation in Ga2O3 is accompanied by substantial jump in conductivity,induced by thermally assisted internal redox reaction of Ga2O3 nanostructure during annealing.It is also experimentally confirmed that the charge transfer in alloxide heterostructures can be tuned and controlled by the heterointerfaces manipulation.Results demonstrate that the engineering of heterointerfaces of two-dimensional(2D)films enables the fabrication of either high-sensitive TiO2–Ga2O3(Ar)or high-threshold TiO2–Ga2O3(N2)nociceptors.The hypersensitive nociceptor mimics the functionalities of corneal nociceptors of human eye,whereas the delayed reaction of nociceptor is similar to high-threshold nociceptive characteristics of human sensory system.The long-term stability of 2D nociceptors demonstrates the capability of heterointerfaces engineering for e ective control of charge transfer at 2D heterostructured devices.

关键词： 2D heterostructures Artificial nociceptors Bio-inspired device heterointerfaces engineering

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Controlled growth of complex polar oxide films with atomically precise molecular beam epitaxy

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Frontiers of physics 2018年第5期13卷 9-21页

作者： Fang Yang Yan Liang Li-Xia Liu Qing Zhu Wei-Hua Wang Xue-Tao Zhu Jian-Dong Guo Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China Collaborative Innovation Center of Quantum Matter Beijing 100871 China

At heterointerfaces between complex oxides with polar discontinuity, the instability-induced electric field may drive electron redistribution, causing a dramatic change in the interracial charge density. This results in the emergence of a rich diversity of exotic physical phenomena in these quasi-two-dimensional systems, which can be further tuned by an external field. To develop novel multifunctional electronic devices, it is essential to control the growth of polar oxide films and heterointerfaces with atomic preci- sion. In this article, we review recent progress in control techniques for oxide film growth by molecular beam epitaxy （MBE）. We emphasize the importance of tuning the microscopic surface structures of polar films for developing precise growth control techniques. Taking the polar SrTiO3 （110） and （111） surfaces as examples, we show that, by keeping the surface reconstructed throughout MBE growth, high-quality layer-by-layer homoepitaxy can be realized. Because the stability of different reconstruc- tions is determined by the surface cation concentration, the growth rate from the Sr/Ti evaporation source can be monitored in real time. A precise, automated control method is established by which insulating homoepitaxial SrTiO3 （110） and （111） films can be obtained on doped metallic substrates. The films show atomically well-defined surfaces and high dielectric performance, which allows the surface carrier concentration to be tuned in the range of -1013/cm2. By applying the knowledge of microstructures from fundamental surface physics to film growth techniques, new opportunities are provided for material science and related research.

关键词： complex oxide films molecular beam epitaxy surface reconstruction heterointerfaces

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NiS2/CoS2/MoS2纳米片阵列:一种高效、廉价的碱性析氢电催化剂

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Science Bulletin 2020年第5期65卷 359-366页

作者：张洋石梦童汪长征朱亚星李念武蒲雄于爱芳翟俊宜 Center for Excellence in Nanoscience Beijing Key Laboratory of Micro-Nano Energy and SensorBeijing Institute of Nanoenergy and NanosystemsChinese Academy of SciencesBeijing 100083China Key Laboratory of Urban Stormwater System and Water Environment(Ministry of Education) Beijing University of Civil Engineering and ArchitectureBeijing 100044China School of Nanoscience and Technology University of Chinese Academy of SciencesBeijing 100049China

大规模高效生产氢气是开发氢能源首先要解决的问题.与酸性条件电解水制取氢气相比,碱性条件下析氢工艺更为成熟且成本较低,具有更广泛的应用前景.如何实现碱性条件下大规模制取氢气,研发高效且廉价的电催化剂是目前能源材料领域的一个... 详细信息

大规模高效生产氢气是开发氢能源首先要解决的问题.与酸性条件电解水制取氢气相比,碱性条件下析氢工艺更为成熟且成本较低,具有更广泛的应用前景.如何实现碱性条件下大规模制取氢气,研发高效且廉价的电催化剂是目前能源材料领域的一个重要课题.通过调整前驱体纳米片阵列中金属钼酸盐的组分,再通过气相硫化,本文实现了过渡金属硫化物纳米片阵列的原位转化.扫描电子显微镜表征证实蜂窝状纳米片阵列的形貌得到了很好的保留,透射电子显微镜表征证实形成了相应的过渡金属硫化物异质结界面.作为碱性析氢电催化剂,具有多种异质结界面的NiS2/CoS2/MoS2纳米片阵列展现出比NiS2/MoS2和CoS2/MoS2纳米片阵列更低的过电位和更小的塔菲尔斜率,并且具有良好的稳定性.本工作展示了构建多重异质结界面在提升催化剂碱性电解水析氢方面的新途径.

关键词： Multiple heterointerfaces In situ conversion Nanosheet array Metal sulfides Hydrogen evolution reaction

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