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A core-shell catalyst design boosts the performance of photothermal reverse water gas shift catalysis

核壳结构增强光热逆水煤气变换催化性能

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Abstract

Photothermal reverse water gas shift (RWGS) catalysis holds promise for efficient conversions of greenhouse gas CO2 and renewable H2, powered solely by sunlight, into CO, an important feedstock for the chemical industry. However, the performance of photothermal RWGS catalysis over existing supported catalysts is limited by the balance between the catalyst loading and dispersity, as well as stability against sintering. Herein, we report a core-shell strategy for the design of photothermal catalysts, by using Ni12P5 as an example, with simultaneously strong light absorption ability, high dispersity and stability. The core-shell structured Ni12P5@SiO2 catalyst with a relatively small Ni12P5 particle size of 15 nm at a high Ni12P5 loading of 30 wt% exhibits improved activity, nearly 100% CO selectivity, and superior stability in photothermal RWGS catalysis, particularly under intense illuminations. Our study clearly reveals the effectiveness of the core-shell strategy in breaking the limitation of supported catalysts and boosting the performance of photothermal CO2 catalysis.

摘要

光热催化逆水煤气变换有望实现完全太阳能驱动条件下, 将 温室气体CO2和可再生H2转化为重要的化工原料CO. 然而现有负 载型光热逆水煤气变换催化剂的性能受限于催化剂负载量、分散 性、稳定性的相互制约. 本文提出了一种核壳结构策略, 并以 Ni12P5为例, 设计了同时具有强光吸收、高分散度和高稳定性的光 热催化剂. 得的Ni12P5@SiO2核壳结构催化剂在Ni12P5负载量高达 30 wt%时, 依然保持了15 nm的较小颗粒尺寸, 从而在光热催化逆 水煤气变换反应中表现出了更高的活性、接近100%的CO选择性 和极佳的稳定性, 尤其是在强光照条件下性能更加突出. 本研究揭 示了核壳策略能有效突破传统负载型催化剂的局限, 提高光热催 化CO2还原的性能.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (51802208, 51920105005, 21902113, 51821002 and 91833303), the Natural Science Foundation of Jiangsu Province (BK20200101), the Collaborative Innovation Centre of Suzhou Nano Science & Technology, and the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). Ozin G is grateful to the Natural Sciences and Engineering Council of Canada for support of this work.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China

    Deyue Lou  (娄德月), Zhijie Zhu  (朱智杰), Chaoran Li  (李超然), Kai Feng  (冯凯), Dake Zhang  (张大科), Kangxiao Lv  (吕康孝), Zhiyi Wu  (吴之怡), Chengcheng Zhang  (张城城), Le He  (何乐) & Xiaohong Zhang  (张晓宏)

  2. Solar Fuels Group, Department of Chemistry, University of Toronto, Toronto, Ontario, M5S 3H6, Canada

    Yang-Fan Xu  (徐杨帆) & Geoffrey A. Ozin

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  1. Deyue Lou  (娄德月)
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  11. Le He  (何乐)
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  12. Xiaohong Zhang  (张晓宏)
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Contributions

He L, Ozin G, Li C and Zhang X conceived and designed the experiments. Lou D, Zhu Z and Xu YF carried out the synthesis of materials. Lv K, Zhang D, Wu Z and Zhang C performed the characterizations. Lou D, Zhu Z and Feng K carried out the catalytic testing. Lou D, Li C, Zhu Z and He L wrote the paper. All the authors contributed to the data analysis, discussed the results, and commented on the manuscript.

Corresponding authors

Correspondence to Chaoran Li  (李超然), Geoffrey A. Ozin or Le He  (何乐).

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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.

Deyue Lou is currently a Master student at FUNSOM, Soochow University. Her research interest focuses on the photothermal catalytic reduction of carbon dioxide.

Zhijie Zhu is currently a PhD student at FUNSOM, Soochow University. His research interest focuses on the photothermal catalytic reduction of carbon dioxide.

Yang-Fan Xu received his Bachelor and PhD degrees from Sun Yat-sen University in 2013 and 2018, respectively. He is now a post-doctoral fellow at the University of Toronto, and his current research interest focuses on the light-driven catalytic CO2 hydrogenation for solar-fuel production.

Chaoran Li received his Bachelor’s degree from Xiamen University and his doctorate degree from Fujian Institute of Research on the Structure of Matter. From 2015 to 2020, he was a postdoctoral researcher at Soochow University. He then joined FUNSOM, Soochow University, as an associate professor. His research interest focuses on controlled synthesis of low-symmetry nanostructures and their applications in photothermal CO2 reduction.

Geoffrey A. Ozin is a Distinguished University Professor at the University of Toronto and the Government of Canada Research Chair in materials chemistry and nanochemistry. He currently spearheads the Solar Fuels Team at the University of Toronto. He has held positions as Honorary Professor at The Royal Institution of Great Britain and University College London, External Adviser for the London Centre for Nanotechnology, Alexander von Humboldt Senior Scientist at the Max Planck Institute for Surface and Colloid Science and the Center for Functional Nanostructures at the Karlsruhe Institute of Technology, and Global Chair at Bath University.

He Le received his Bachelor’s degree from Nanjing University and his doctorate degree from the University of California Riverside. From 2013 to 2015, he was a postdoctoral researcher at the University of Toronto, Canada. In 2015, he joined FUNSOM, Soochow University as a professor. His main research interest focuses on the development of functional nanostructured materials for various demanding applications, especially heterogeneous CO2 photocatalysis.

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Lou, D., Zhu, Z., Xu, YF. et al. A core-shell catalyst design boosts the performance of photothermal reverse water gas shift catalysis. Sci. China Mater. 64, 2212–2220 (2021). https://doi.org/10.1007/s40843-020-1630-2

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