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Near-infrared absorbing 2D/3D ZnIn2S4/N-doped graphene photocatalyst for highly efficient CO2 capture and photocatalytic reduction

具有近红外吸收的二维/三维ZnIn2S4/氮掺杂石墨烯光催化剂的制备及其高效 CO2 捕获和光催化还原性能

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Abstract

Hierarchical heterostructure photocatalysts with broad spectrum solar light utilization, particularly in the near-infrared (NIR) region, are emerging classes of advanced photocatalytic materials for solar-driven CO2 conversion into value-added chemical feedstocks. Herein, a novel two-demensional/three-demensional (2D/3D) hierarchical composite is hydrothermally synthesized by assembling vertically-aligned ZnIn2S4 (ZIS) nanowall arrays on nitrogen-doped graphene foams (NGF). The prepared ZIS/NGF composite shows enhancement in photothermal conversion ability and selective CO2 capture as well as solar-driven CO2 photoreduction. At 273 K and 1 atm, the ZIS/NGF composite with 1.0 wt% NGF achieves a comparably high CO2-to-N2 selectivity of 30.1, with an isosteric heat of CO2 adsorption of 48.2 kJ mol−1. And in the absence of cocatalysts and sacrificial agents, the ZIS/NGF composite with cyclability converts CO2 into CH4, CO and CH3OH under simulated solar light illumination, with the respective evolution rates about 9.1, 3.5, and 5.9 times higher than that of the pristine ZIS. In-depth analysis using in-situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) in conjunction with Kelvin probe measurements reveals the underlying charge transfer pathway and process from ZIS to NGF.

摘要

具有宽光谱太阳能利用的分等级异质结光催化剂, 正成为一种新兴的先进光催化材料, 被应用于太阳能驱动二氧化碳转化为高附加值的化学原料. 本工作通过水热法使二维硫化铟锌纳米墙垂直生长于三维氮掺杂石墨烯泡沫上, 形成分等级异质结光催化剂. 该催化剂展现出优异的光热转换效率、选择性捕获CO2和光催化还原CO2的能力. 在273 K和1个大气压条件下, 负载1 wt% 氮掺杂石墨烯泡沫的复合催化剂表现出最优异的性能, 其中对CO2和N2的吸附选择性为30.1, 并且对CO2的等量吸附热为48.2 kJ mol−1. 在无助催化剂和牺牲剂的条件下, 负载1 wt% 氮掺杂石墨烯泡沫的复合催化剂, 其光催化转化CO2为CH4、 CO和 CH3OH的效率分别是纯的硫化铟锌的9.1、 3.5和5.9倍. 该增强效应得益于三维石墨烯泡沫高度开放的网状结构, 良好的CO2吸附能力和两种组份之间的强相互作用. 此外, 利用原位照射X射线光电子能谱仪和开尔文探针技术分析了电荷转移的方向, 本工作为设计高效太阳能转化分等级异质结光催化剂开辟了新的思路.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51961135303, 51932007, 21871217 and U1705251), the National Key Research and Development Program of China (2018YFB1502001) and Innovative Research Funds of SKLWUT (2017-ZD-4).

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Authors and Affiliations

  1. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China

    Yang Xia  (夏阳), Bei Cheng  (程蓓) & Jiaguo Yu  (余家国)

  2. School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China

    Jiajie Fan  (范佳杰) & Jiaguo Yu  (余家国)

  3. CAS Key Laboratory of Standardization and Measurement for Nanotechnology, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing, 100190, China

    Gang Liu  (刘刚)

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  1. Yang Xia  (夏阳)
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  2. Bei Cheng  (程蓓)
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  3. Jiajie Fan  (范佳杰)
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  4. Jiaguo Yu  (余家国)
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Contributions

Yu J, Liu G and Xia Y conceived and designed the experiments. Xia Y carried out the synthesis of the materials and photocatalytic test. Xia Y, Fan J and Cheng B performed the material characterizations. Xia Y, Yu J and Liu G contributed to data analysis. Yu J, Liu G and Cheng B supervised the project. Yu J, Liu G and Xia Y wrote the paper. All authors discussed the results and commented on the manuscript.

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Correspondence to Jiaguo Yu  (余家国) or Gang Liu  (刘刚).

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The authors declare that they have no conflict of interest.

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Supporting data are available in the online version of the paper.

Yang Xia received his MS degree from South Central University for Nationalities in 2017. He is now a PhD candidate under the supervision of Prof. Jiaguo Yu at the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology. His current research includes semi-conductor photocatalysis, photocatalytic H2 production, and CO2 reduction.

Jiaguo Yu received his BS and MS degrees in chemistry from Central China Normal University and Xi’an Jiaotong University, respectively, and his PhD degree in materials science in 2000 from Wuhan University of Technology. In 2000, he became a Professor at Wuhan University of Technology. His current research interests include semiconductor photocatalysis, photocatalytic hydrogen production, CO2 reduction to hydrocarbon fuels, and so on.

Gang Liu received his PhD degree in 2000 from Texas A&M University, USA. Then he did his postdoctoral work at Brookhaven National Laboratory, University of Pennsylvania and Temple University. He joined the National Center for Nanoscience and Technology, China, in 2007 as an associate professor. His research interests lie in the characterization and properties of a variety of nanoscale materials important in environmental control and clean energy production.

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Near-infrared absorbing 2D/3D ZnIn2S4/N-doped graphene photocatalyst for highly efficient CO2 capture and photocatalytic reduction

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Xia, Y., Cheng, B., Fan, J. et al. Near-infrared absorbing 2D/3D ZnIn2S4/N-doped graphene photocatalyst for highly efficient CO2 capture and photocatalytic reduction. Sci. China Mater. 63, 552–565 (2020). https://doi.org/10.1007/s40843-019-1234-x

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