Abstract：
Advanced photocatalysts are highly desired to activate the photocatalytic CO2reduction reaction (CO2RR) with low concentration. Herein, the NiSn(OH)6with rich surface lattice hydroxyls was synthesized to boost the activity directly under the natural air. Results showed that terminal Ni-OH could serve as donors to feed protons and generate oxygen vacancies (VO), thus beneficial to convert the activated CO2(HCO3-) mainly into CO (5.60μmol g-1) in the atmosphere. It was flexible and widely applicable for a stable CO2RR from high pure to air level free of additionally adding H2O reactant, and higher than the traditional gas-liquid-solid (1.58μmol g-1) and gas-solid (4.07μmol g-1) reaction system both using high pure CO2and plenty of H2O. The strong hydrophilia by the rich surface hydroxyls allowed robust H2O molecule adsorption and dissociation at VOsites to achieve the Ni-OH regeneration, leading to a stable CO yield (11.61μmol g-1) with the enriched renewable VOregardless of the poor CO2and H2O in air. This work opens up new possibilities for the practical application of natural photosynthesis.
摘要：
高度期望先进的光催化剂以低浓度活化光催化CO2还原反应(CO2RR)。在这里，合成了具有丰富表面晶格羟基的NiSn（OH）6，以直接在自然空气中增强活性。结果表明，末端Ni-OH可以作为供体供给质子并产生氧空位（VO），从而有利于将大气中的活化CO2(HCO3-)主要转化为CO(5.60μmol/g)。它是灵活的，广泛适用于从高纯到空气水平的稳定的CO2RR，没有额外添加H2O反应物，高于传统的气-液-固（1.58μmol/g）和气-固（4.07μmol/g）反应体系，均使用高纯CO2和大量H2O。丰富的表面羟基的强亲水性使H2O分子在VO位点的强大吸附和解离实现Ni-OH再生，无论空气中的CO2和H2O含量如何，富含可再生VO都会导致稳定的CO产量（11.61μmol/g）。这项工作为自然光合作用的实际应用开辟了新的可能性。
