刘琦, 窦燕青, 巩宙婷, 刘守军, 陈亮宇, 陶钰文, 刘晋芳, 杨颂. 氟掺杂在碳辅助电解水制氢中强化碳氧化反应研究[J]. 燃料化学学报(中英文). DOI: 10.1016/S1872-5813(24)60474-3
引用本文: 刘琦, 窦燕青, 巩宙婷, 刘守军, 陈亮宇, 陶钰文, 刘晋芳, 杨颂. 氟掺杂在碳辅助电解水制氢中强化碳氧化反应研究[J]. 燃料化学学报(中英文). DOI: 10.1016/S1872-5813(24)60474-3
LIU Qi, DOU Yanqing, GONG Zhouting, LIU Shoujun, CHEN Liangyu, TAO Yuwen, LIU Jinfang, YANG Song. Research on improving carbon oxidation by fluorine doping in carbon-assisted water electrolysis for hydrogen production[J]. Journal of Fuel Chemistry and Technology. DOI: 10.1016/S1872-5813(24)60474-3
Citation: LIU Qi, DOU Yanqing, GONG Zhouting, LIU Shoujun, CHEN Liangyu, TAO Yuwen, LIU Jinfang, YANG Song. Research on improving carbon oxidation by fluorine doping in carbon-assisted water electrolysis for hydrogen production[J]. Journal of Fuel Chemistry and Technology. DOI: 10.1016/S1872-5813(24)60474-3

氟掺杂在碳辅助电解水制氢中强化碳氧化反应研究

Research on improving carbon oxidation by fluorine doping in carbon-assisted water electrolysis for hydrogen production

  • 摘要: 面临着“双碳”目标的约束,氢能,尤其是电解水制氢技术受到了广泛的关注。然而,高能耗是制约该技术产业化的关键问题之一。基于此,提出“牺牲阳极碳辅助电解水制氢”的策略,利用碳氧化反应(COR)替代析氧反应(OER),实现能耗的大幅降低。具体是利用两步碳化法制备出F掺杂生物炭(记作F-BC-850),采用XRD、SEM-EDS、热重分析、XPS等表征手段解析F-BC-850的结构特征;通过电化学方法阐明F-BC-850与制氢性能间的构效关系。结果表明,在0.5 mol/L H2SO4溶液中,10 mA/cm2下,其能耗是传统Pt片电极的57.9%;表征结果表明,氟化铵热解产生的HF刻蚀生物炭,能够形成活性较强的C−F键,进而提升了碳氧化性能。F物种的引入改变了碳结构,促进H2O分子产生*OH,并强化了碳原子对*OH的吸附能力。本工作可为碳辅助电解水制氢高效产H2和生物质高值化利用提供科学依据。

     

    Abstract: Faced with the constraints of the “carbon peaking and carbon neutrality goals”, the electrolysis of water for hydrogen production has received significant attention. However, high energy consumption is one of the problems hindering the industrialization of the technology. A strategy for “sacrificial anode carbon-assisted electrolysis of water for hydrogen production” is thus proposed, which uses the carbon oxidation reaction (COR) instead of the oxygen evolution reaction (OER) to achieve a significant reduction in energy consumption. In particular, F-doped biochar (denoted as F-BC-850) was prepared using a simple two-step carbonization method. The structural properties were analyzed using XRD, SEM-EDS, thermogravimetric, XPS and other characterization techniques. The structure-activity relationship was elucidated by electrochemical tests. The results showed that the energy consumption in 0.5 mol/L H2SO4 solution at 10 mA/cm2 was 57.9% of the conventional Pt sheet electrode. Characterization results showed that HF generated by the pyrolysis of ammonium fluoride etched the biochar and formed highly active C−F bonds, which improved the oxidation performance of carbon. The addition of F species changed the carbon structure, promoted the decomposition of H2O molecules to *OH radicals, and thus increased the adsorption ability of carbon atoms for *OH radicals. This work can provide theoretical guidelines for the efficient production of H2 by carbon-assisted electrolysis of water and high-quality utilization of biomass.

     

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