电合成
材料科学
化学工程
镍
无定形固体
过氧化氢
纳米技术
电化学
有机化学
冶金
化学
电极
物理化学
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,Zhenhui Kang
标识
DOI:10.1002/adma.202202995
摘要
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 (H2 O2 ). 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 Ni2+ with different amounts of BH4- . Among borides, the amorphous NiB2 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 H2 O2 production rate of 4.753 mol gcat-1 h-1 is achieved upon assembling NiB2 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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