题目: | phase reconstruction-directed synthesis of oxalate-functionalized nickel hydroxide electrocatalyst for high-yield h2o2 generation at industrial currents |
作者: | zhiwei liu1, weijie yuan1, hongyuan yang2, zhenhui kang1*, mengjie ma1, prashanth w. menezes2,3* & ziliang chen1,3* |
单位: | 1institute of functional nano & soft materials (funsom), jiangsu key laboratory for carbon-based functional materials & devices, soochow university, 199 ren’ai road, suzhou, jiangsu 215123, china. 2department of chemistry: metalorganics and inorganic materials technische universität berlin, straße des 17 juni 135, sekr. c2, 10623 berlin, germany. 3material chemistry group for thin film catalysis–catlab helmholtz-zentrum berlin für materialien und energie, albert-einstein-str. 15, 12489 berlin, germany. |
摘要: | the electrochemical oxygen reduction reaction (2e− orr) offers a promising approach for h2o2 production, yet developing highly active, selective, and stable electrocatalysts remains a challenge. in this work, a phase reconstruction strategy is presented to synthesize an oxalate-adsorbed nickel hydroxide electrocatalyst (ni(oh)2-c2o4) through the self-dissociation of nickel oxalate in an alkaline medium, leading to a notable enhancement in h2o2 yield at elevated current densities. remarkably, ni(oh)2-c2o4 exhibits a 2e− selectivity exceeding 93% across a broad voltage range (0.0 to 0.5 v vs. rhe) in 0.1 m koh, outperforming pristine ni(oh)2. when deployed as a gas diffusion electrode in a flow cell, the ni(oh)2-c2o4 catalyst demonstrates stable operation for 50 h at 200 ma cm−2, with a faradaic efficiency surpassing 90% and a peak h2o2 yield of 6.2 mol g−1cat h−1. comprehensive advanced characterizations, including in situ raman spectroscopy, transient photovoltage spectra, and transient potential scanning spectra, coupled with post-orr analyses, reveal that surface-adsorbed oxalate groups on ni(oh)2 enhance the interfacial reaction kinetics between active ni sites and reactants by inducing a charge trapping effect and forming a hydrogen-bonded network, facilitating robust and high-yield h2o2 production. |
影响因子: | 18.5 |
分区情况: | 一区 |
链接: | 责任编辑:杜欣 |