Vertical graphene array for efficient electrocatalytic reduction of oxygen to hydrogen peroxide

石墨烯 材料科学 法拉第效率 过氧化氢 电极 电化学 催化作用 可逆氢电极 化学气相沉积 化学工程 电催化剂 纳米技术 工作电极 有机化学 化学 物理化学 工程类
作者
Yulin Wang,Run Shi,Lu Shang,Lishan Peng,Dewei Chu,Zhaojun Han,Geoffrey I. N. Waterhouse,Rui Zhang,Tierui Zhang
出处
期刊:Nano Energy [Elsevier BV]
卷期号:96: 107046-107046 被引量:63
标识
DOI:10.1016/j.nanoen.2022.107046
摘要

Hydrogen peroxide (H 2 O 2 ) is a green chemical oxidant that finds widespread use in the chemical industry. The electrocatalytic oxygen reduction reaction (ORR) is presently attracting a lot of attention as an environmentally friendly synthetic route towards H 2 O 2 . However, the efficient reduction of O 2 to produce H 2 O 2 at high current densities (> 100 mA cm −2 ), thereby achieving viable H 2 O 2 yields, remains a challenge. Herein, we demonstrate that vertical graphene arrays grown on carbon paper (denoted herein as VG array) via plasma-enhanced chemical vapor deposition show outstanding activity for ORR to H 2 O 2 in alkaline media at high current densities. The VG array electrode delivered a Faradaic efficiency of 94% and a H 2 O 2 production rate of 61.3 mg h −1 cm −2 at 100 mA cm −2 , and similarly impressive performance at 200 mA cm −2 (81% and 102.8 mg cm −2 h −1 , respectively), outperforming most catalysts reported to date for electrochemical H 2 O 2 synthesis. The remarkable performance of the VG array electrode is ascribed to the interconnected network of graphene nanosheets which ensures a high availability of graphene edge active sites (thus a high H 2 O 2 selectivity) and fast electron transfer during ORR. Further, gas-liquid-solid three-phase interfaces formed between the graphene nanosheets facilitate a steady supply of O 2 from the gas phase when the electrode was applied in a flow cell. Results encourage the application array electrodes in electrochemical H 2 O 2 synthesis, whilst also offering a roadmap to future industrial H 2 O 2 production. • The vertical graphene array (VG array) delivered a high faradaic efficiency and H 2 O 2 production rate at large current densities (100 and 200 mA cm −2 ). • TheVG array ensured high availability of graphene edge active sites and fast electron transfer during ORR. • The VG array possessed abundant gas-liquid-solid interfaces, which promoted efficient O 2 supply from the gas phase to the catalytic sites.
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