Amine functionalized surface frustrated Lewis pairs boost CO2 photocatalysis†‡

EES catalysis Pub Date : 2024-01-09 DOI:10.1039/D3EY00261F
Qinhui Guan, Chengzhe Ni, Tingjiang Yan, Na Li, Lu Wang, Zhe Lu, Weiguang Ran, Yipin Zhang, Wenjuan Li, Lulu Zhang, Dapeng Zhang, Baibiao Huang and Geoffrey A. Ozin
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Abstract

The archetype surface frustrated Lewis pair (SFLP) that facilitates CO2 photocatalytic hydrogenation to methanol and carbon monoxide, is an InOH⋯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⋯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.

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胺官能化表面受挫路易斯对促进二氧化碳光催化
促进二氧化碳光催化加氢生成甲醇和一氧化碳的典型表面挫折路易斯对(SFLP)是位于纳米级氢氧化铟(In2O3-x(OH)y)表面的InOH--In位点。这种类型的近端路易斯酸 In(III) 和路易斯碱 InOH 可作为表面活性位点,促成光化学异解 H2 和将 CO2 还原成上述产物。研究发现,光的转化率远远超过热的转化率。为了提高 SFLP 的 CO2 光催化性能,需要通过用 Bi(III)同构取代 In(III)来改变路易斯酸度和碱性,并通过控制氧化物的非全度来改变氧空位的数量。用更强的路易斯碱胺 InNH2 取代路易斯碱氢氧化物 InOH 的研究至今仍未进行。本文所述的探索这一机遇的策略始于 In2O3-x(EDA)y 的合成。事实证明,这种新材料含有 InNH2-In SFLP,其二氧化碳光催化性能优于其 In2O3-x(OH)y 原合物。量身定制的路易斯酸性和碱性表面使二氧化碳光催化离太阳能二氧化碳精炼厂的愿景又近了一步。
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Back cover Correction: High photocatalytic yield in the non-oxidative coupling of methane using a Pd–TiO2 nanomembrane gas flow-through reactor Embedding the intermetallic Pt5Ce alloy in mesopores through Pt–C coordination layer interactions as a stable electrocatalyst for the oxygen reduction reaction† Efficient CO2-to-CO conversion in dye-sensitized photocatalytic systems enabled by electrostatically-driven catalyst binding† Green energy driven methane conversion under mild conditions
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