Structure-controlled graphene electrocatalysts for high-performance H2O2 production,Energy & Environmental Science

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Structure-controlled graphene electrocatalysts for high-performance H2O2 production
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2022-05-19 , DOI: 10.1039/d2ee00548d
Kyungbin Lee ₁ , Jeonghoon Lim ₁ , Michael J. Lee ₁ , Kun Ryu ₁ , Hoyoung Lee ₁ , Jin Young Kim ₂ , Hyunchul Ju ₃ , Hyun-Seok Cho ₄ , Byung-Hyun Kim ₅ , Marta C. Hatzell ₁ , Joonhee Kang _{5,

6} , Seung Woo Lee ₁

Affiliation

Metal-free carbon materials have emerged as cost-effective and high-performance catalysts for the production of hydrogen peroxide (H₂O₂) through the two-electron oxygen reduction reaction (ORR). Here, we show that 3D crumpled graphene with controlled oxygen and defect configurations significantly improves the electrocatalytic production of H₂O₂. The crumpled graphene electrocatalyst with optimal defect structures and oxygen functional groups exhibits outstanding H₂O₂ selectivity of 92–100% in a wide potential window of 0.05–0.7 V vs. reversible hydrogen electrode (RHE) and a high mass activity of 158 A g⁻¹ at 0.65 V vs. RHE in alkaline media. In addition, the crumpled graphene catalyst showed an excellent H₂O₂ production rate of 473.9 mmol gcat⁻¹ h⁻¹ and stability over 46 h at 0.4 V vs. RHE. Moreover, density functional theory calculations revealed the role of the functional groups and defect sites in the two-electron ORR pathway through the scaling relation between OOH and O adsorption strengths. These results establish a structure-mechanism-performance relationship of functionalized carbon catalysts for the effective production of H₂O₂.

中文翻译：

用于高性能 H2O2 生产的结构控制石墨烯电催化剂

无金属碳材料已成为通过双电子氧还原反应 (ORR)生产过氧化氢 (H ₂ O ₂ )的经济高效的高性能催化剂。在这里，我们展示了具有可控氧和缺陷配置的 3D 皱褶石墨烯显着改善了 H ₂ O ₂的电催化生产。具有最佳缺陷结构和氧官能团的皱褶石墨烯电催化剂在 0.05-0.7 V与可逆氢电极 (RHE)的宽电位窗口中表现出 92-100% 的出色 H ₂ O ₂选择性和 158 A 的高质量活性g ^-1在 0.65 V与碱性介质中的 RHE 相比。此外，皱褶的石墨烯催化剂表现出优异的 H ₂ O ₂产率，为 473.9 mmol gcat ^-1 h ^-1和 0.4 V vs. RHE下 46 小时内的稳定性。此外，密度泛函理论计算通过 OOH 和 O 吸附强度之间的比例关系揭示了官能团和缺陷位点在双电子 ORR 途径中的作用。这些结果建立了功能化碳催化剂的结构-机理-性能关系，以有效生产 H ₂ O ₂。

更新日期：2022-05-19

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