Reductive Transformation of Layered-Double-Hydroxide Nanosheets to Fe-Based Heterostructures for Efficient Visible-Light Photocatalytic Hydrogenation of CO

Yufei Zhao; Zhenhua Li; Mengzhu Li; Jinjia Liu; Xingwu Liu; Geoffrey I N Waterhouse; Yuanshen Wang; Jiaqing Zhao; Wa Gao; Zhaosheng Zhang; Run Long; Qinghua Zhang; Lin Gu; Xi Liu; Xiaodong Wen; Ding Ma; Li-Zhu Wu; Chen-Ho Tung; Tierui Zhang

doi:10.1002/adma.201803127

Reductive Transformation of Layered-Double-Hydroxide Nanosheets to Fe-Based Heterostructures for Efficient Visible-Light Photocatalytic Hydrogenation of CO

Adv Mater. 2018 Jul 31:e1803127. doi: 10.1002/adma.201803127. Online ahead of print.

Authors

Yufei Zhao¹, Zhenhua Li^{1

2}, Mengzhu Li³, Jinjia Liu^{4

5}, Xingwu Liu^{4

5}, Geoffrey I N Waterhouse⁶, Yuanshen Wang^{1

2}, Jiaqing Zhao^{1

2}, Wa Gao³, Zhaosheng Zhang⁷, Run Long⁷, Qinghua Zhang⁸, Lin Gu⁸, Xi Liu^{4

5}, Xiaodong Wen^{4

5}, Ding Ma³, Li-Zhu Wu¹, Chen-Ho Tung¹, Tierui Zhang^{1

9}

Affiliations

¹ Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
² Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of the Ministry of Education, College of Chemistry & Materials Science, Northwest University, Xi'an, 710127, China.
³ College of Chemistry and Molecular Engineering and College of Engineering, BIC-ESAT, Peking University, Beijing, 100871, China.
⁴ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China.
⁵ Synfuels China, Beijing, 100195, China.
⁶ School of Chemical Sciences, The University of Auckland, Auckland, 1142, New Zealand.
⁷ College of Chemistry, Key Laboratory of Theoretical and Computational Photochemistry of Ministry of Education, Beijing Normal University, Beijing, 100875, China.
⁸ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
⁹ University of Chinese Academy of Sciences, Beijing, 100049, China.

PMID: 30066491
DOI: 10.1002/adma.201803127

Abstract

Conversion of syngas (CO, H₂ ) to hydrocarbons, commonly known as the Fischer-Tropsch (FT) synthesis, represents a fundamental pillar in today's chemical industry and is typically carried out under technically demanding conditions (1-3 MPa, 300-400 °C). Photocatalysis using sunlight offers an alternative and potentially more sustainable approach for the transformation of small molecules (H₂ O, CO, CO₂ , N₂ , etc.) to high-valuable products, including hydrocarbons. Herein, a novel series of Fe-based heterostructured photocatalysts (Fe-x) is successfully fabricated via H₂ reduction of ZnFeAl-layered double hydroxide (LDH) nanosheets at temperatures (x) in the range 300-650 °C. At a reduction temperature of 500 °C, the heterostructured photocatalyst formed (Fe-500) consists of Fe⁰ and FeO_x nanoparticles supported by ZnO and amorphous Al₂ O₃ . Fe-500 demonstrates remarkable CO hydrogenation performance with very high initial selectivities toward hydrocarbons (89%) and especially light olefins (42%), and a very low selectivity towards CO₂ (11%). The intimate and abundant interfacial contacts between metallic Fe⁰ and FeO_x in the Fe-500 photocatalyst underpins its outstanding photocatalytic performance. The photocatalytic production of high-value light olefins with suppressed CO₂ selectivity from CO hydrogenation is demonstrated here.

Keywords: CO hydrogenation; Fe-based catalysts; layered double hydroxides; light olefins; photocatalysis.