在中性 pH 条件下通过稳定的大环镍(II)配合物进行均相电催化水氧化。
Homogeneous electrocatalytic water oxidation at neutral pH by a robust macrocyclic nickel(II) complex.
机构信息
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, State Key Laboratory of Optoelectronic Materials and Technologies, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275 (China).
出版信息
Angew Chem Int Ed Engl. 2014 Nov 24;53(48):13042-8. doi: 10.1002/anie.201406983. Epub 2014 Sep 9.
The development of an earth-abundant, first-row water oxidation catalyst that operates at neutral pH and low overpotential remains a fundamental chemical challenge. Herein, we report the first nickel-based robust homogeneous water oxidation catalyst, which can electrocatalyze water oxidation at neutral pH and low overpotential in phosphate buffer. The results of DFT calculations verify that the O-O bond formation in catalytic water oxidation prefers a HO-OH coupling mechanism from a cis-isomer of the catalyst.
开发一种在中性 pH 值和低过电势下工作的丰富地球元素、第一行水氧化催化剂仍然是一个基本的化学挑战。在此，我们报告了首例镍基坚固的均相水氧化催化剂，它可以在磷酸盐缓冲液中在中性 pH 值和低过电势下电催化水氧化。DFT 计算的结果验证了在催化水氧化中 O-O 键的形成更倾向于催化剂顺式异构体的 HO-OH 偶联机制。
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