Engineered disorder in CO2 photocatalysis

Zhao Li, Chengliang Mao, Qijun Pei, Paul N. Duchesne, Teng He, Meikun Xia, Jintao Wang, Lu Wang, Rui Song, Feysal M. Ali, Débora Motta Meira, Qingjie Ge, Kulbir Kaur Ghuman (), Le He, Xiaohong Zhang () and Geoffrey A. Ozin ()
Additional contact information
Zhao Li: Soochow University
Chengliang Mao: University of Toronto
Qijun Pei: Chinese Academy of Sciences
Paul N. Duchesne: Queen’s University
Teng He: Chinese Academy of Sciences
Meikun Xia: University of Toronto
Jintao Wang: Chinese Academy of Sciences
Lu Wang: The Chinese University of Hong Kong, Shenzhen
Rui Song: Soochow University
Feysal M. Ali: University of Toronto
Débora Motta Meira: Argonne National Laboratory
Qingjie Ge: Chinese Academy of Sciences
Kulbir Kaur Ghuman: Matériaux et Télécommunications
Le He: Soochow University
Xiaohong Zhang: Soochow University
Geoffrey A. Ozin: University of Toronto

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Light harvesting, separation of charge carriers, and surface reactions are three fundamental steps that are essential for an efficient photocatalyst. Here we show that these steps in the TiO2 can be boosted simultaneously by disorder engineering. A solid-state reduction reaction between sodium and TiO2 forms a core-shell c-TiO2@a-TiO2-x(OH)y heterostructure, comprised of HO-Ti-[O]-Ti surface frustrated Lewis pairs (SFLPs) embedded in an amorphous shell surrounding a crystalline core, which enables a new genre of chemical reactivity. Specifically, these SFLPs heterolytically dissociate dihydrogen at room temperature to form charge-balancing protonated hydroxyl groups and hydrides at unsaturated titanium surface sites, which display high reactivity towards CO2 reduction. This crystalline-amorphous heterostructure also boosts light absorption, charge carrier separation and transfer to SFLPs, while prolonged carrier lifetimes and photothermal heat generation further enhance reactivity. The collective results of this study motivate a general approach for catalytically generating sustainable chemicals and fuels through engineered disorder in heterogeneous CO2 photocatalysts.

Date: 2022
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DOI: 10.1038/s41467-022-34798-1

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