Huang Yuming, Zhou Wei, Xie Liang, Meng Xiaoxiao, Li Junfeng, Gao Jihui, Zhao Guangbo, Qin Yukun
School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, People's Republic of China.
Proc Natl Acad Sci U S A. 2024 Nov 19;121(47):e2316352121. doi: 10.1073/pnas.2316352121. Epub 2024 Nov 14.
Electrooxidation of renewable and CO-neutral biomass for low-cost hydrogen production is a promising and green technology. Various biomass platform molecules (BPMs) oxidation assisted hydrogen production technologies have obtained noticeable progress. However, BPMs anodic oxidation is highly dependent on electrocatalysts, and the oxidation mechanism is ambiguous. Meanwhile, the complexity and insolubility of natural biomass severely constrain the efficient utilization of biomass resources. Here, we develop a self-sacrificing and self-supporting carbon anode (SSCA) using waste corncobs. The combined results from multiple characterizations reveal that the structure-property-activity relationship of SSCA in carbon oxidation reaction (COR). Theoretical calculations demonstrate that carbon atoms with a high spin density play a pivotal role in reducing the adsorption energy of the reactive oxygen intermediate (*OH) during the transition from OH to *OH, thereby promoting COR. Additionally, the HER||COR system allows driving a current density of 400 [Formula: see text] at 1.24 V at 80 °C, with a hydrogen production electric consumption of 2.96 kWh Nm (H). The strategy provides a ground-breaking perspective on the large-scale utilization of biomass and low-energy water electrolysis for hydrogen production.
通过可再生且碳中性的生物质进行电氧化以低成本制氢是一项很有前景的绿色技术。各种生物质平台分子（BPMs）氧化辅助制氢技术已取得显著进展。然而，BPMs的阳极氧化高度依赖于电催化剂，且氧化机理尚不明确。同时，天然生物质的复杂性和不溶性严重制约了生物质资源的高效利用。在此，我们利用废弃玉米芯开发了一种自牺牲且自支撑的碳阳极（SSCA）。多种表征的综合结果揭示了SSCA在碳氧化反应（COR）中的结构-性质-活性关系。理论计算表明，具有高自旋密度的碳原子在从OH转变为*OH的过程中，对于降低活性氧中间体（*OH）的吸附能起着关键作用，从而促进COR。此外，HER||COR系统在80°C、1.24 V时可驱动400[公式：见原文]的电流密度，制氢电耗为2.96 kWh Nm（H）。该策略为生物质的大规模利用和低能耗水电解制氢提供了开创性的视角。
