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Co3O4 Nanocrystals with Oxygen Vacancy-Rich and Highly Reactive (222) Facet on Carbon Nitride Scaffolds for Efficient Photocatalytic Oxygen Evolution.
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-09-13 , DOI: 10.1021/acsami.0c09761
Yunxiong Zeng 1 , Hao Li 2 , Yingchun Xia 1 , Longlu Wang 1 , Kai Yin 1 , Yuanfeng Wei 1 , Xia Liu 1 , Shenglian Luo 1
Affiliation  

Oxygen evolution reaction (OER) with sluggish kinetics is the rate-determining step of water splitting, which dominates the solar-to-hydrogen fuel conversion efficiency. Herein, we constructed an oxygen vacancy-rich and highly reactive (222) facet in Co3O4 nanocrystals anchored on carbon nitride nanofiber (CNF) by a solvothermal reduction method. The resulting Co3O4 nanocrystals/CNF (COCNF) demonstrated a dramatically enhanced OER with a rate of 24.9 μmol/h under visible light, which is 124 times higher than that of CNF. This excellent catalytic activity of COCNF is based on a synergistic effect between its binary components for charge separation, oxygen vacancies for enhanced conductivity, and facet (222) exposure of Co3O4 nanocrystals for improved heterogeneous kinetics. Density functional theory (DFT) calculations revealed the water oxidation mechanism at different facets and found that the formed oxygen vacancies lead to a reduction of the materials’ bandgap. The correlation between Co3O4 crystal facets and the inherent OER catalytic activities under acidic solution was in the order of (222) > (220) > (311).

中文翻译:

具有高氧空位和高反应性(222)刻面的氮化碳支架上的Co3O4纳米晶体,可有效释放光催化的氧气。

动力学缓慢的氧气析出反应(OER)是水分解的决定速率的步骤,它决定着太阳能到氢燃料的转化效率。在这里,我们通过溶剂热还原法在锚定在氮化碳纳米纤维(CNF)上的Co 3 O 4纳米晶体中构造了一个富氧空位和高反应性的(222)刻面。所得的Co 3 O 4纳米晶体/ CNF(COCNF)在可见光下显示出显着增强的OER,速率为24.9μmol/ h,是CNF的124倍。COCNF的这种出色的催化活性是基于其二元组分用于电荷分离,氧空位以增强电导率以及Co的小平面(222)暴露之间的协同效应。3 O 4纳米晶体可改善异质动力学。密度泛函理论(DFT)的计算揭示了水在不同方面的氧化机理,并发现形成的氧空位导致材料带隙的减小。在酸性溶液中,Co 3 O 4晶面与固有的OER催化活性之间的相关性依次为(222)>(220)>(311)。
更新日期:2020-10-07
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