Amine functionalized surface frustrated Lewis pairs boost CO2 photocatalysis

被引：12

作者：

Guan, Qinhui ^{[1
]}

Ni, Chengzhe ^{[1
]}

Yan, Tingjiang ^{[1
,2
]}

Li, Na ^{[1
,3
]}

Wang, Lu ^{[4
]}

Lu, Zhe ^{[4
]}

Ran, Weiguang ^{[1
]}

Zhang, Yipin ^{[1
]}

Li, Wenjuan ^{[1
]}

Zhang, Lulu ^{[1
]}

Zhang, Dapeng ^{[1
]}

Huang, Baibiao ^{[3
]}

Ozin, Geoffrey A. ^{[5
]}

机构：

[1] Qufu Normal Univ, Sch Chem & Chem Engn, Key Lab Catalyt Convers & Clean Energy Univ Shando, Qufu 273165, Peoples R China

[2] Shaanxi Univ Sci & Technol, Coll Chem & Chem Engn, Xian 710021, Peoples R China

[3] Shandong Univ, State Key Lab Crystal Mat, Jinan 250100, Peoples R China

[4] Chinese Univ Hong Kong, Sch Sci & Engn, Shenzhen 518172, Guangdong, Peoples R China

[5] Univ Toronto, Dept Chem, Mat Chem & Nanochem Res Grp, Solar Fuels Cluster, 80 St George St, Toronto, ON M5S 3H6, Canada

来源：

EES CATALYSIS | 2024年 / 2卷 / 02期

基金：

中国国家自然科学基金; 加拿大自然科学与工程研究理事会;

关键词：

MODIFIED SBA-15; CARBON-DIOXIDE; INDIUM OXIDE; ADSORBED CO2; HYDROGENATION; EFFICIENT; FTIR; METHANOL; SILICAS; XPS;

D O I：

10.1039/d3ey00261f

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The archetype surface frustrated Lewis pair (SFLP) that facilitates CO2 photocatalytic hydrogenation to methanol and carbon monoxide, is an InOH & ctdot;In site positioned in the surface of a nanoscale indium oxide hydroxide, denoted In2O3-x(OH)y. Proximal Lewis acid In(iii) and Lewis base InOH of this genre serve as surface active sites that enable the photochemical heterolytic H2 dissociation and reduction of CO2 to the mentioned products. The conversion rate enabled by light has been found to far exceed that enabled by heat. Efforts to enhance the CO2 photocatalytic performance of the SFLP have involved modifications of the Lewis acidity and basicity through isomorphic substitution of In(iii) with Bi(iii) and changes in the population of oxygen vacancies through control of oxide non-stoichiometry. Replacement of the Lewis base hydroxide InOH by the stronger Lewis base amine InNH2 heretofore remains unexplored. The strategy described herein to explore this opportunity begins with the synthesis of In2O3-x(EDA)y. This new material is proven to contain an InNH2 & ctdot;In SFLP and its CO2 photocatalytic performance is demonstrated to outperform that of its In2O3-x(OH)y progenitor. Tailored Lewis acidity and basicity surfaces bring CO2 photocatalysis another step closer to the vision of solar CO2 refineries.

引用

页码：573 / 584

页数：13

共 69 条

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