Zhang Lu, Kong Ling-Yi, Zhang Xin, Zhou Xiao-Cheng, Feng Jiu-Ju, Wang Ai-Jun
Key laboratory of the Ministry of Education for Advanced Catalysis Materials, College of Chemistry and Materials Science, College of Geography and Environmental Sciences, Zhejiang Normal University, Jinhua, Zhejiang, 321004, P. R. China.
Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, Jiangsu Key Laboratory of New Power Batteries, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, Jiangsu, 210023, P. R. China.
Small. 2024 Oct;20(40):e2402981. doi: 10.1002/smll.202402981. Epub 2024 Jun 5.
To address the imperative challenge of producing hydrogen in a low-energy consumption electrocatalytic system, this study emphasizes the utilization of thermodynamically favorable biomass oxidation for achieving energy-efficient hydrogen generation. This research integrates ultralow PtO-loaded flower-like nanosheets (denoted as PtO@CuO/Cu FNs) with Cu/Cu pairs and Pt─O bonds, thereby yielding substantial enhancement in both hydrogen evolution reaction (HER, -0.042 V at 10 mA cm) and furfural oxidation reaction (FFOR, 0.09 V at 10 mA cm). As validated by DFT calculations, the dual built-in electric field (BIEF) is elucidated as the driving force behind the enhanced activities, in which Pt─O bonds expedite the HER, while Cu/Cu promotes low-potential FFOR. By coupling the FFOR and HER together, the resulting bipolar-hydrogen production system requires a low power input (0.5072 kWh per m) for producing H. The system can generate bipolar hydrogen and high value-added furoic acid, significantly enhancing hydrogen production efficiency and concurrently mitigating energy consumption.
为应对在低能耗电催化系统中制氢这一紧迫挑战,本研究着重利用热力学有利的生物质氧化来实现高效节能的氢气生成。本研究将超低负载量的PtO负载的花状纳米片(记为PtO@CuO/Cu FNs)与Cu/Cu对以及Pt─O键相结合,从而在析氢反应(HER,在10 mA cm时为-0.042 V)和糠醛氧化反应(FFOR,在10 mA cm时为0.09 V)中均产生显著增强。经密度泛函理论(DFT)计算验证,双内置电场(BIEF)被阐明为活性增强背后的驱动力,其中Pt─O键加速HER,而Cu/Cu促进低电位FFOR。通过将FFOR和HER耦合在一起,所得的双极制氢系统生产氢气所需的功率输入较低(每立方米0.5072 kWh)。该系统可产生双极氢气和高附加值的糠酸,显著提高制氢效率并同时降低能耗。