Yan Tingjiang, Li Na, Wang Linlin, Ran Weiguang, Duchesne Paul N, Wan Lili, Nguyen Nhat Truong, Wang Lu, Xia Meikun, Ozin Geoffrey A
The Key Laboratory of Life-Organic Analysis, College of Chemistry and Chemical Engineering, Qufu Normal University, 273165, Qufu, Shandong, People's Republic of China.
Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON, M5S 3H6, Canada.
Nat Commun. 2020 Nov 30;11(1):6095. doi: 10.1038/s41467-020-19997-y.
The surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H and CO molecules and enable efficient gas-phase CO photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In ions in InO by single-site Bi ions, thereby enhancing the propensity to activate CO molecules. The so-formed BiInO materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than InO itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of BiInO also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO photocatalysis, another step towards the vision of the solar CO refinery.
负载缺陷的金属氧化物表面的受阻路易斯酸碱对（SFLPs）提供了催化位点，可激活H和CO分子，并实现高效的气相CO光催化。金属氧化物的晶格工程为调整SFLPs的反应活性提供了一种有用的策略。在此，开发了一种一步溶剂热合成法，该方法能够通过单位点Bi离子对InO中的路易斯酸位点In离子进行同构取代，从而增强激活CO分子的倾向。如此形成的BiInO材料在逆水煤气变换反应中的光活性比InO本身高三个数量级，同时对甲醇生产也表现出显著的光活性。BiInO提高的太阳能吸收效率以及有效的电荷分离和转移也有助于改善光催化性能。这些特性例证了在多相CO光催化中进行原子尺度工程的机会，这是朝着太阳能CO精炼厂愿景迈出的又一步。
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