Electro-oxidation of 5-hydroxymethylfurfural by a catalyst containing copper nanoparticles and single copper atoms

Materials Today Catalysis Pub Date : 2024-01-23 DOI:10.1016/j.mtcata.2024.100041

Yongfang Zhou , Yi Shen , Hongying Li

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Abstract

Atomic-site electrocatalysts are being considered as potential alternative catalysts due to their exceptionally high atom utilization efficiencies, well-defined active sites and high selectivities. However, the presence of nanoparticles in the single-atom catalysts may affect the catalytic performance. Herein, single-copper-atoms and copper nanoparticles co-embedded in nitrogen-doped carbon nanosheets (Cu_NPs@Cu/NCNSs) were synthesized for 5-hydroxymethylfurfural electro-oxidation. Single copper atoms supported on nitrogen-doped carbon nanosheets (Cu/NCNSs) and copper nanoparticles supported on carbon (Cu_NPs/C) were also synthesized for comparison. The Cu_NPs/C exhibited high efficiency in electro-oxidation of HMF to 2,5-furandicarboxylic acid (FDCA) at a low potential of 1.42 V. However, the Cu_NPs@Cu/NCNSs showed a high 5-formyl-2-furancarboxylic acid (FFCA) selectivity of 86.7%. Oxalic acid (OA) treatment experiments showed that single copper atoms played a major role on the oxidation of HMF to FFCA. Cu(OH)₂ active species generated by electrochemical oxidation were demonstrated as the primary catalytic sites for HMF oxidation on the Cu_NPs/C. In-situ Raman spectra results demonstrated that HMF oxidation on the Cu_NPs/C followed the path to 5-hydroxymethyl-2-furancarboxylic acid (HFCA), while on the Cu_NPs@Cu/NCNSs and Cu/NCNSs, HMF was oxidized along the 5-diformylfuran (DFF) pathway.

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含纳米铜颗粒和单个铜原子的催化剂对 5-羟甲基糠醛的电氧化作用

原子位点电催化剂因其极高的原子利用效率、明确的活性位点和高选择性而被视为潜在的替代催化剂。然而，单原子催化剂中纳米颗粒的存在可能会影响催化性能。在此，研究人员合成了单铜原子和纳米铜粒子共同嵌入掺氮碳纳米片（CuNPs@Cu/NCNSs），用于 5- 羟甲基糠醛电氧化。为了进行比较，还合成了支撑在掺氮碳纳米片（Cu/NCNSs）上的单个铜原子和支撑在碳上的铜纳米颗粒（CuNPs/C）。在 1.42 V 的低电位下，CuNPs/C 在将 HMF 电氧化成 2,5-呋喃二甲酸 (FDCA) 的过程中表现出很高的效率。草酸（OA）处理实验表明，单个铜原子在将 HMF 氧化成 FFCA 的过程中发挥了重要作用。电化学氧化产生的 Cu(OH)2 活性物种被证明是 CuNPs/C 上 HMF 氧化的主要催化位点。原位拉曼光谱结果表明，HMF 在 CuNPs/C 上的氧化路径是 5-羟甲基-2-呋喃羧酸（HFCA），而在 CuNPs@Cu/NCNSs 和 Cu/NCNSs 上，HMF 的氧化路径是 5-二甲酰呋喃（DFF）。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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