Chen Guangyu, Fu Cenfeng, Zhang Wenhua, Gong Wanbing, Ma Jun, Ji Xiaomin, Qian Lisheng, Feng Xuefei, Hu Chuansheng, Long Ran, Xiong Yujie
School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, National Synchrotron Radiation Laboratory, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, PR China.
School of Materials Science and Engineering, Hefei University of Technology, Hefei, Anhui, PR China.
Nat Commun. 2025 Jan 14;16(1):665. doi: 10.1038/s41467-025-56094-4.
Solar-driven, selective biomass hydrogenation is recognized as a promising route to renewable chemicals production, but remains challenging. Here, we report a TiO supported Cu single-atom catalyst with a four-coordinated Cu-O structure, which can be universally applied for solar-driven production of various renewable chemicals from lignocellulosic biomass-derived platform molecules with good yields using green methanol as a hydrogen donor, to address this challenge. It is significant that the biomass upgrading driven by natural sunlight on a gram scale demonstrates the great practical potential. By combining in situ soft X-ray absorption spectroscopy with theoretical calculations, we successfully identify the dynamic evolution of Cu sites along with the biomass hydrogenation and methanol oxidation, where the tandem process is enabled by the photogenerated electrons and holes to complete a chemical cycle. The concept of solar-driven biomass hydrogenation proposed here provides an efficient and sustainable methodology for the sustainable production of renewable chemicals.
太阳能驱动的选择性生物质加氢被认为是生产可再生化学品的一条有前途的途径，但仍然具有挑战性。在此，我们报道了一种具有四配位Cu-O结构的TiO负载的Cu单原子催化剂，它可以普遍应用于以绿色甲醇为氢供体，从木质纤维素生物质衍生的平台分子中太阳能驱动生产各种可再生化学品，并具有良好的产率，以应对这一挑战。重要的是，在克级规模上由自然阳光驱动的生物质升级展示了巨大的实际潜力。通过将原位软X射线吸收光谱与理论计算相结合，我们成功地确定了Cu位点随生物质加氢和甲醇氧化的动态演变，其中串联过程由光生电子和空穴驱动以完成一个化学循环。这里提出的太阳能驱动生物质加氢的概念为可再生化学品的可持续生产提供了一种高效且可持续的方法。
