Liu Boxin, Hu Zhuofeng, Li Yanfang, Tan Xin, Ye Jinhua, Yu Tao
School of Environmental Science and Engineering, Tianjin University, Tianjin, P. R. China.
School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou, P. R. China.
Nat Commun. 2025 Jul 1;16(1):6014. doi: 10.1038/s41467-025-61223-0.
The biggest challenge facing the advancement of photocatalytic technology so far is how to achieve the simultaneous and efficient utilization of photogenerated electrons and holes for dual value-added chemicals. Here we show that Pd/TiO with electronic metal-support interaction realizes photocatalytic HO evolution coupled with furfural selective oxidation to furoic acid. We demonstrate that the electronic structure of Pd is modulated to form Pd active sites and upshifted d-band center via electronic metal-support interaction, enhancing O adsorption and HO evolution performance, and the photogenerated holes from TiO oxidize furfural undergoing the Aldehyde-Water Shift to furoic acid by sequential breaking of O-H and C-H bonds. The optimal Pd/TiO achieves HO and furoic acid evolution rates of 3672.31 and 4529.08 μM h with furfural conversion of 92.66% and furoic acid selectivity of 97.82%. Our work provides a promising approach for enhancing synergistic photosynthesis of dual value-added chemicals, thus advancing carbon neutrality goals.
迄今为止，光催化技术发展面临的最大挑战是如何实现光生电子和空穴同时高效地用于合成两种高附加值化学品。在此，我们展示了具有电子金属-载体相互作用的Pd/TiO实现了光催化析氢，同时将糠醛选择性氧化为糠酸。我们证明，通过电子金属-载体相互作用，Pd的电子结构被调制以形成Pd活性位点并使d带中心上移，增强了O吸附和析氢性能，并且来自TiO的光生空穴通过依次断裂O-H和C-H键，将糠醛氧化为糠酸，这一过程经历了醛-水转移反应。最优的Pd/TiO实现了析氢和糠酸生成速率分别为3672.31和4529.08 μM h，糠醛转化率为92.66%，糠酸选择性为97.82%。我们的工作为增强两种高附加值化学品的协同光合作用提供了一种有前景的方法，从而推动碳中和目标的实现。
