通过优化电子调制†，增强了ce掺杂nipxe上的电催化析氢反应、析氧反应和生物质氧化

IF 9.2 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2025-05-28 DOI:10.1039/d5gc01605c

Shuhan Liu , Yifei Ye , Lele Gao , Zhen Yan , Haokun Pan , Zhaokun Wang , Guangrui Zhang , Xiubing Huang

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引用次数: 0

摘要

利用高效电催化剂电催化氧化5-羟甲基糠醛（HMFOR）制2,5-呋喃二羧酸（FDCA）是目前的研究热点。本研究采用一步电化学沉积法合成了泡沫镍负载的ce掺杂过渡金属磷化物（即Ce-NiPx/NF）。Ce的Lewis酸性为含氧底物提供了吸附位点，而Ni的电子结构由于其价态的变化可以有效地调整。此外，Ce和P的电荷调制促进了Ni的快速增值，反应过程中P的逸出形成了许多氧空位，有利于HMF的吸附。在电流密度为10 mA cm−2时，析氢反应（HER）和析氧反应（OER）的过电位分别为116 mV和276 mV。对于HMFOR，在1.40 VRHE条件下，HMF转化率接近100%，FDCA产率和法拉第效率分别为98.69%和98.38%，循环20次后均保持在95%以上。本研究提出了一种简便的构建电催化氧化还原杂原子电极的方法，为设计高性能电催化剂提供了一种方法。

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Enhanced electrocatalytic hydrogen evolution reaction, oxygen evolution reaction and biomass oxidation over Ce-doped NiPxvia optimization of electronic modulation†

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR) to 2,5-furandicarboxylic acid (FDCA) using highly efficient electrocatalysts is currently a research hotspot. In this study, nickel foam-supported Ce-doped transition metal phosphide (i.e., Ce-NiP_x/NF) was synthesized using a one-step electrochemical deposition method. The Lewis acidity of the Ce species offered adsorption sites for oxygen-containing substrates, and the electronic structure of Ni could be effectively adjusted due to its variable valence state. In addition, the charge modulation of Ce and P promoted the rapid valorization of Ni, and the escape of P during the reaction formed many oxygen vacancies, which facilitated the adsorption of HMF. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) required overpotentials of only 116 mV and 276 mV for a current density of 10 mA cm⁻², respectively. For HMFOR, the HMF conversion reached almost 100%, and the FDCA yield and Faraday efficiency were 98.69% and 98.38% at 1.40 V_RHE, respectively, and both remained above 95% after 20 cycles. This study presents a facile method for constructing heteroatomic electrodes for electrocatalytic oxidation and reduction and provides a method for designing high-performance electrocatalysts.

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.