材料科学
化学工程
镍
无定形固体
拉曼光谱
过氧化氢
选择性
溶解
催化作用
有机化学
冶金
化学
物理
光学
工程类
作者
Jie Wu,Meilin Hou,Ziliang Chen,Weiju Hao,Xuelei Pan,Hongyuan Yang,Wanglai Cen,Yang Liu,Hui Huang,Prashanth W. Menezes
标识
DOI:10.1002/adma.202202995
摘要
Abstract Developing advanced electrocatalysts with exceptional two electron (2e − ) selectivity, activity, and stability is crucial for driving the oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O 2 ). Herein, a composition engineering strategy is proposed to flexibly regulate the intrinsic activity of amorphous nickel boride nanoarchitectures for efficient 2e − ORR by oriented reduction of Ni 2+ with different amounts of BH 4 − . Among borides, the amorphous NiB 2 delivers the 2e − selectivity close to 99% at 0.4 V and over 93% in a wide potential range, together with a negligible activity decay under prolonged time. Notably, an ultrahigh H 2 O 2 production rate of 4.753 mol g cat −1 h −1 is achieved upon assembling NiB 2 in the practical gas diffusion electrode. The combination of X‐ray absorption and in situ Raman spectroscopy, as well as transient photovoltage measurements with density functional theory, unequivocally reveal that the atomic ratio between Ni and B induces the local electronic structure diversity, allowing optimization of the adsorption energy of Ni toward *OOH and reducing of the interfacial charge‐transfer kinetics to preserve the OO bond.
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