作者：

Wenjing Zhang^1#, Xuewei Hao^1#, Xinlin Liu¹, Mingyu Chu¹, Shengming Li¹, Xuchun Wang³, Feng Jiang⁴, Lu Wang¹*, Qiao Zhang¹, Jinxing Chen¹*, Dingsheng Wang², and Muhan Cao¹*

单位：

¹Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, 215123, People's Republic of China.

²Engineering Research Center of Advanced Rare Earth Materials, Department of Chemistry, Tsinghua University, Beijing, 100084, People's Republic of China.

³X-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States.

⁴School of Minerals Processing and Bioengineering, Central South University, Changsha, 410083, People's Republic of China.

摘要：

Photoreforming presents a promising strategy for upcycling waste polyester-derived alcohol into valuable chemicals. However, it remains a great challenge due to its low performance and unsatisfactory selectivity toward high-value C₂ products. Here, we report the highly efficient and selective conversion of ethylene glycol (EG, a monomer of polyethylene terephthalate (PET)) to glycolaldehyde using atomically dispersed Pd species supported on TiO₂ catalyst. A glycolaldehyde production rate of 5072 μmol g_cat^-1h^-1 with a selectivity of 90.0% and long-term durability can be achieved. Experimental and theoretical results show that Pd single atoms can enhance the photocatalytic activity by enriching the photogenerated holes, which are the dominant species for the selective oxidation of EG to glycolaldehyde. More importantly, the adsorption of EG molecules on the catalysts is significantly promoted, which is subsequently transformed into RO• radicals, a crucial intermediate in producing glycolaldehyde. Additionally, Pd single atoms on TiO₂ enable the reduction of the glycolaldehyde desorption barrier, thereby facilitating high selectivity and inhibiting further oxidation to C₁ products. This work provides new insights into the photocatalytic conversion of polyester wastes by atomic engineering.

影响因子：

16.1

分区情况：

一区

链接：

https://doi.org/10.1002/anie.202500814

责任编辑：杜欣