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in-plane heterostructured Ag_(2)S-In_(2)S_(3) atomic layers enabling boosted CO_(2) photoreduction into CH_(4)

Nano Research 2021年第12期14卷 4520-4527页

作者： Weiwei Shao Shumin Wang Juncheng Zhu Xiaodong Li Xingchen Jiao Yang Pan Yongfu Sun Yi Xie Hefei National Laboratory for Physical Sciences at Microscale CAS Centre for Excellence in NanoscienceNational Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei230026China Institute of Energy Hefei Comprehensive National Science CenterHefei230031China

Sluggish separation and migration kinetics of the photogenerated carriers account for the low-efficiency of CO_(2) photoreduction into CH_(4). Design and construction two-dimensional (2D) in-plane heterostructures demonstrate to be an appealing approach to address above obstacles. Herein, we fabricate 2D in-plane heterostructured Ag_(2)S-In_(2)S_(3) atomic layers via an ion-exchange strategy. Photoluminescence spectra, time-resolved photoluminescence spectra, and photoelectrochemical measurements firmly affirm the optimized carrier dynamics of the In_(2)S_(3) atomic layers after the introduction of in-plane heterostructure. In-situ Fourier transform infrared spectroscopy spectra and density functional theory (DFT) calculations disclose the in-plane heterostructure contributes to CO_(2) activation and modulates the adsorption strength of CO* intermediates to facilitate the formation of CHO* intermediates, which are further protonated to CH4. In consequence, the in-plane heterostructure achieves the CH_(4) evolution rate of 20 µmol·g^(−1)·h^(−1), about 16.7 times higher than that of the In2S3 atomic layers. In short, this work proves construction of in-plane heterostructures as a promising method for obtaining high-efficiency CO_(2)-to-CH_(4) photoconversion properties.

关键词： in-plane heterostructure atomic layers carrier dynamics selective CO_(2)photoreduction

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In situ electrochemical dehydrogenation of ultrathin Co(OH)_(2) nanosheets for enhanced hydrogen evolution

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Chinese Chemical Letters 2023年第1期34卷 469-473页

作者： Qian Zhou Qihang Bian Liling Liao Fang Yu Dongyang Li Dongsheng Tang Haiqing Zhou Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of EducationKey Laboratory for Matter Microstructure and Function of Hunan ProvinceHunan Normal UniversityChangsha 410081China Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy Hunan UniversityChangsha 410082China

Transition metal hydroxides/oxyhydroxides have recently emerged as highly active electrocatalysts for oxygen evolution reaction in alkaline water electrolysis,while have not yet been widely investigated for hydrogen evolution electrocatalysts owing to their unfavorable H*-adsorption,making it difficult to construct an overall-water-splitting cell for hydrogen *** this work,we proposed a straightforward and effective approach to develop an efficient in-plane heterostructured CoOOH/Co(OH)_(2) catalyst via in-situ electrochemical dehydrogenation method,in which the dehydrogenated–CoOOH and Co(OH)_(2) at the surface synergistically boost the hydrogen evolution reaction(HER)kinetics in base as confirmed by high-resolution transmission electron microscope,synchrotron X-ray absorption spectroscopy,and electron energy loss *** to the in-situ dehydrogenation of ultrathin Co(OH)_(2) nanosheets,the catalytic activity of the CoOOH/Co(OH)_(2) heterostructures is progressively improved,which exhibit outstanding hydrogen-evolving activity in base requiring a low overpotential of 132 m V to afford 10 m A/cm^(2)with very fast reaction kinetics after 60 h *** gradually improved catalytic performance for the CoOOH/Co(OH)2is probably due to the enhanced H*-adsorption induced by the synergistic effect of heterostructures and better conductivity of Co OOH relative to electrically insulating Co(OH)_(2).This work will open the opportunity for a new family of transition metal hydroxides/oxyhydroxides as active HER catalysts,and also highlight the importance of using in situ techniques to construct precious metal-free efficient catalysts for alkaline hydrogen evolution.

关键词： Hydrogen evolution reaction Transition metal hydroxide In-situ electrochemical dehydrogenation in-plane heterostructure Water splitting

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