Defying the oxidative-addition prerequisite in cross-coupling through artful single-atom catalysts
Heterogeneous single-atom catalysts (SACs) have gained significant attention for their maximized atom utilization and well-defined active sites, but they often struggle with multi-stage organic cross-coupling reactions due to limited coordination space and reactivity. Here, we report an "anchoring-borrowing" strategy combined facet engineering to develop artful single-atom catalysts (ASACs) through anchoring foreign single atoms onto specific facets of the non-innocent reducible carriers. ASACs exhibit adaptive coordination, effectively bypassing the oxidative-addition prerequisite for bivalent elevation at a single metal site in both homogenous and heterogeneous cross-couplings. For example, Pd<sub>1</sub>-CeO<sub>2</sub>(110) ASAC exhibits unparalleled activity in coupling with more accessible aryl chlorides, and challenging heterocycles, outperforming traditional catalysts with a remarkable turnover number of 45,327,037. Mechanistic studies reveal that ASACs leverage dynamic structural changes, with reducible carriers acting as electron reservoirs, significantly lowering reaction barriers. Furthermore, ASACs enable efficient synthesis of biologically significant compounds, drug intermediates, and active pharmaceutical ingredients (APIs) through a scalable high-speed circulated flow synthesis, underscoring great potential for sustainable fine chemical manufacturing.
Authors
- Xingjie Fu
- Jinghan Li (ORCID: https://orcid.org/0000-0003-3619-5121)
- Lu Ma (ORCID: https://orcid.org/0000-0001-9646-0738)
- Xiao Hai (ORCID: https://orcid.org/0000-0002-7631-9769)
- Yifan Xu (ORCID: https://orcid.org/0000-0002-0153-7761)
- Yudong Yang (ORCID: https://orcid.org/0000-0002-7142-2249)
- Huihui Lin (ORCID: https://orcid.org/0000-0002-1971-3380)
- Quan‐Hong Yang (ORCID: https://orcid.org/0000-0003-2882-3968)
- Shibo Xi (ORCID: https://orcid.org/0000-0002-8521-3237)
- Jie Wu (ORCID: https://orcid.org/0000-0002-9865-180X)
- Gang Wang (ORCID: https://orcid.org/0000-0001-6857-5415)
- Dongshuang Wu (ORCID: https://orcid.org/0000-0001-8512-8473)
- Qian He (ORCID: https://orcid.org/0000-0003-4891-3581)
- Jiong Lu (ORCID: https://orcid.org/0000-0002-3690-8235)
- Rongwei Meng (ORCID: https://orcid.org/0000-0002-9874-0909)
- Jiwei Shi (ORCID: https://orcid.org/0000-0003-3625-9324)
- Peng He (ORCID: https://orcid.org/0000-0002-7141-4660)
- Yu Teng (ORCID: https://orcid.org/0009-0005-7339-7605)
- Duanshuai Tian
- Xin Zhou (ORCID: https://orcid.org/0000-0002-6431-731X)
- Jun Li (ORCID: https://orcid.org/0000-0002-8456-3980)
- Hengyu Li (ORCID: https://orcid.org/0009-0007-1906-0520)
- Qilong Cai (ORCID: https://orcid.org/0000-0003-3932-702X)
- Jinxing Chen (ORCID: https://orcid.org/0009-0007-8666-4586)
- Jiali Li (ORCID: https://orcid.org/0000-0001-8990-9998)
- Yang‐Gang Wang (ORCID: https://orcid.org/0000-0002-0582-0855)
Institutions
- Agency for Science, Technology and Research (SG)
- Tianjin University (CN)
- National University of Singapore (SG)
- Nanyang Technological University (SG)
- Brookhaven National Laboratory (US)
- Peking University (CN)
- Southern University of Science and Technology (CN)
- Suzhou University of Science and Technology (CN)
- Suzhou Research Institute (CN)
- Collaborative Innovation Center of Chemical Science and Engineering Tianjin (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-04-04
- DOI
- https://doi.org/10.1038/s41467-025-58579-8
- Citations
- 17
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 6.18
Funders
- Agency for Science, Technology and Research
- Government of Jiangsu Province
- Ministry of Education, India
- Southern University of Science and Technology
- Science and Technology Support Program of Jiangsu Province