Large low-field magnetic enhancement in photoredox hydrodechlorination of N-heteroarene chlorides restricted by poor cage escape.
7 affiliations
- 1Spin-X Institute, School of Chemistry and Chemical Engineering, Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 511442, China.
- 2College of Chemistry, Beijing Normal University, Beijing 100875, China.
- 3Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.
- 4College of Science, National University of Defense Technology, Changsha 410003, China.
- 5South China Advanced Institute for Soft Matter Science and Technology, Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou 510641, China.
- 6Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education, School of Chemistry, LIFM, IGCME, GBRCE for Functional Molecular Engineering, Sun Yat-sen University, Guangzhou 510275, China.
- 7Beijing National Laboratory of Molecular Science, Beijing Key Laboratory of Magnetoelectric Materials and Devices, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Abstract
The efficiency of photoredox catalysis has long been hampered by rapid back electron transfer (BET) within the radical ion pairs (RIPs). While external magnetic fields can modulate the spin dynamics of RIPs to suppress BET, achieving a large magnetic field effect (MFE) at low field strengths has remained a formidable challenge. Herein, we report a remarkably large MFE, with a quantum yield enhancement exceeding 130% and a yield enhancement up to 160%, in the photoredox hydrodechlorination of N-heteroaryl chlorides under a weak magnetic field. This enhancement arises from the effective magnetic field modulation of the hyperfine-coupling-driven spin dynamics within triplet-born RIPs, particularly for systems with poor cage escape. By reversely applying a kinetic model developed in our previous work, we successfully deconvolve complex reaction pathways and quantitatively reproduce the intrinsic magnetic sensitivity, reconciling experimental observations with theoretical predictions in terms of half-saturation field. This work provides a new paradigm for photoredox transformation through spin modulation and demonstrates practical synthetic utility at high conversions, offering a powerful strategy for enhancing catalytic efficiency through accessible magnetic fields.
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BibTeX
@article{sun2026large,
title = {{Large low-field magnetic enhancement in photoredox hydrodechlorination of N-heteroarene chlorides restricted by poor cage escape.}},
author = {Mingli Sun and Chenli Chen and Lingfang Chen and Shen Zhou and Jianyu Liu and Binghui Xue and Panchao Yin and Jiayi Liang and Shuming Bai and Jialong Jie and Hongmei Su and Song Gao and Linan Zhou},
journal = {National science review},
year = {2026},
month = jul,
doi = {10.1093/nsr/nwag450},
url = {https://europepmc.org/article/MED/42953317},
note = {CC BY},
}
RIS
TY - JOUR
TI - Large low-field magnetic enhancement in photoredox hydrodechlorination of N-heteroarene chlorides restricted by poor cage escape.
AU - Mingli Sun
AU - Chenli Chen
AU - Lingfang Chen
AU - Shen Zhou
AU - Jianyu Liu
AU - Binghui Xue
AU - Panchao Yin
AU - Jiayi Liang
AU - Shuming Bai
AU - Jialong Jie
AU - Hongmei Su
AU - Song Gao
AU - Linan Zhou
PY - 2026
DA - 2026/07/24
JO - National science review
DO - 10.1093/nsr/nwag450
UR - https://europepmc.org/article/MED/42953317
AB - The efficiency of photoredox catalysis has long been hampered by rapid back electron transfer (BET) within the radical ion pairs (RIPs). While external magnetic fields can modulate the spin dynamics of RIPs to suppress BET, achieving a large magnetic field effect (MFE) at low field strengths has remained a formidable challenge. Herein, we report a remarkably large MFE, with a quantum yield enhancement exceeding 130% and a yield enhancement up to 160%, in the photoredox hydrodechlorination of N-heteroaryl chlorides under a weak magnetic field. This enhancement arises from the effective magnetic field modulation of the hyperfine-coupling-driven spin dynamics within triplet-born RIPs, particularly for systems with poor cage escape. By reversely applying a kinetic model developed in our previous work, we successfully deconvolve complex reaction pathways and quantitatively reproduce the intrinsic magnetic sensitivity, reconciling experimental observations with theoretical predictions in terms of half-saturation field. This work provides a new paradigm for photoredox transformation through spin modulation and demonstrates practical synthetic utility at high conversions, offering a powerful strategy for enhancing catalytic efficiency through accessible magnetic fields.
SN - 2095-5138
SN - 2053-714X
ER -