Unveiling the Gold Facet Effect in Selective Oxidation of 5-Hydroxymethylfurfural and Hydrogen Production
Direct oxidation of 5-hydroxymethylfurfural (HMF) to 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), crucial for medical supply production, is hindered by overoxidation. We synthesized gold nanomaterials with distinct single-crystal facets, {111} in octahedra (OC), {100} in nanocubes (NCs), and {110} in rhombic dodecahedra (RD), to investigate the facet-dependent HMF oxidation. The Au RD achieved the spontaneous oxidation of HMF to HMFCA with stoichiometric hydrogen production, maintaining 95% carbon balance, 91% yield, and 98% selectivity. In contrast, Au OC and NCs were inert. The superior performance is due to the absence of a C-H activation energy barrier on the Au(110) facet. Furthermore, gas chromatography and isotope experiments supported that the intermediate is oxidized to produce H<sub>2</sub> via H<sup>-</sup> transfer, rather than H<sub>2</sub>O via H<sup>+</sup> transfer. Oxygen was essential for scavenging electrons, thereby closing the reaction loop. The Au RD exhibited remarkable stability, operating for 240 h without performance degradation, indicating its potential for efficient HMFCA production.
Authors
- Xuehao Sun
- Haixin Lin (ORCID: https://orcid.org/0000-0003-4650-0062)
- Renfeng Liu
- Sheng Dai (ORCID: https://orcid.org/0000-0001-5787-0179)
- Guangxu Chen (ORCID: https://orcid.org/0000-0002-8670-4708)
- Yun Zhao (ORCID: https://orcid.org/0000-0001-6003-3136)
- An Pei (ORCID: https://orcid.org/0000-0002-5000-6414)
- Qiqi Wu (ORCID: https://orcid.org/0000-0002-7034-3864)
- Tan Li (ORCID: https://orcid.org/0000-0003-2803-4539)
- Hongpeng He (ORCID: https://orcid.org/0000-0002-0033-3214)
- Qingfeng Zhang (ORCID: https://orcid.org/0000-0002-7004-9040)
- Fan Gao (ORCID: https://orcid.org/0009-0006-7518-3835)
- Yanyan Jia (ORCID: https://orcid.org/0000-0001-7089-0959)
- Qizhen Qin
- Peng Wang (ORCID: https://orcid.org/0000-0003-1824-2545)
Institutions
- Kunming University of Science and Technology (CN)
- East China University of Science and Technology (CN)
- Xiamen University (CN)
- Wuhan University (CN)
- State Key Laboratory of Luminescent Materials and Devices
- South China University of Technology (CN)
Publication Details
- Journal
- Nano Letters
- Published
- 2024-12-11
- DOI
- https://doi.org/10.1021/acs.nanolett.4c04786
- Citations
- 14
- Primary Topic
- Catalysis for Biomass Conversion
- Type
- article
- Field-Weighted Citation Impact
- 2.58
Funders
- National Natural Science Foundation of China
- Ministry of Science and Technology of the People's Republic of China
- Natural Science Foundation of Guangdong Province
- Guangdong Provincial Pearl River Talents Program
- Guangzhou Municipal Science and Technology Project