Yang Shilin, Miao Jingyu, Hou Nannan, Liu Minghui, Jing Baojian, Zhang Jiayu, Qiu Shan, Deng Fengxia
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China.
Contemporary Amperex Technology Limited, Ningde, 352100, China.
Small. 2025 Apr;21(17):e2500499. doi: 10.1002/smll.202500499. Epub 2025 Mar 27.
The sustainable production of hydrogen peroxide (HO) via the two-electron oxygen reduction reaction (2e⁻ ORR) on carbon-based catalysts offers a compelling alternative to the energy-intensive anthraquinone process. However, the slow kinetics of the 2e⁻ ORR in acidic media limits its efficiency. Herein, a novel strategy is introduced to overcome this limitation by engineering a needle-shaped hydrophobic carbon felt embedded with hard carbon as a natural air diffusion electrode (ADE). In situ and ex situ characterization show this design creates an oxygen-enriched, locally alkaline microenvironment at the triphase interface, which accelerates 2e⁻ ORR kinetics by confining oxygen enrichment within the hard carbon layer. Quantitatively, this oxygen-enriched hydrothermal carbon electrocatalyst achieves a remarkable HO selectivity of 95.47% at near-zero overpotential and a high production rate of 487.82 mg L h at 200 mA cm. Furthermore, density functional theory calculations reveal that the carboxyl and ether functional groups in hydrothermal hard carbon optimize O and OOH adsorption, promoting the desired 2e⁻ pathway. Importantly, this ADE design not only exhibits exceptional performance and long-term stability but also demonstrates a significantly reduced global warming potential compared to conventional methods, highlighting its potential to revolutionize industrial-scale HO electrosynthesis by replacing commercial carbon black-based cathodes.
通过碳基催化剂上的双电子氧还原反应（2e⁻ ORR）可持续生产过氧化氢（HO），为能源密集型蒽醌法提供了一个有吸引力的替代方案。然而，酸性介质中2e⁻ ORR的缓慢动力学限制了其效率。在此，引入了一种新策略来克服这一限制，即设计一种嵌入硬碳的针状疏水碳毡作为天然空气扩散电极（ADE）。原位和非原位表征表明，这种设计在三相界面处创造了一个富氧的局部碱性微环境，通过将氧富集限制在硬碳层内来加速2e⁻ ORR动力学。定量地说，这种富氧水热碳电催化剂在接近零过电位时实现了95.47%的显著HO选择性，在200 mA cm下具有487.82 mg L h的高产率。此外，密度泛函理论计算表明，水热硬碳中的羧基和醚官能团优化了O和OOH的吸附，促进了所需的2e⁻途径。重要的是，这种ADE设计不仅表现出优异的性能和长期稳定性，而且与传统方法相比，其全球变暖潜力显著降低，突出了其通过取代商业炭黑基阴极来革新工业规模HO电合成的潜力。
