| Autor: |
Xie, Shangfang, Fu, Hongchuan, Chen, Liyu, Li, Yingwei, Shen, Kui |
| Zdroj: |
SCIENCE CHINA Chemistry; 20230101, Issue: Preprints p1-12, 12p |
| Abstrakt: |
The electrooxidation of 5-hydroxymethylfurfural (HMFOR) not only offers a green route to attain high-value 2,5-furandicarboxylic acid (FDCA) from biomass, but also is considered as a promising approach to replace the kinetically sluggish OER for future hydrogen production. Herein, we report the construction and structural optimization of Ce-doped ultrasmall Co2P nanoparticles (NPs) in carbon-based nanoarrays to boost HER-coupled HMFOR. We demonstrate that the electronic structure of Co-based electrocatalysts can be positively regulated by Ce doping and the optimized Ce-Co2P-based electrocatalyst only require a low voltage of 1.20 V vs.RHE to achieve 10 mA cm−2for HMFOR with an excellent FDCA Faraday efficiency (FEFDCA) of 98.5%, which are superior to its Ce-free counterpart (1.29 V vs.RHE; FEFDCA=83.9 %). When being assembled into a HER-coupled HMFOR system, this bifunctional electrocatalyst can achieve 50 mA cm−2with an ultralow voltage of 1.46 V, which is reduced by 210 mV as compared with that of its Ce-free counterpart (1.67 V). Quasi-operandoexperiments and DFT calculations further reveal the significant roles of Ce doping in promoting the charge transfer between active sites and HMF, and reducing the free energy barrier of intermediate (*HMFCA) dehydrogenation. This study provides new insights into the underlying mechanisms of Ce doping into metal phosphides for boosting HER-coupled HMFOR, developing a facile methodology to construct efficient electrocatalysts for energy storage/conversion systems. |
| Databáze: |
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