作者：

Xinge Hu^1#, Jinjie Liu^2#, Zhijie Zhu^1#, Shuang Liu^1#, Lei Wang¹, Jianjun Cheng³, Xiong Huang³, Chaoran Li¹, Kai Feng¹, Yuxuan Zhou¹, Yuqing Xu¹, Qianyue Feng¹, Binbin Zhang⁴, Xiankai Chen¹, Liang Zhang¹, Qingfeng Zhang⁴, Bo Wu³*, Jun Yin²*, Xingda An¹*, Xiao-Hong Zhang¹* & Le He¹*

摘要：

Light-mediated electronic spin modulation possesses intriguing potentials for photochemistry, enabling on-demand customization of catalysts towards distinct reactions and catalytic requirements. However, the significant photobleaching of the transient spin transitions as well as their temporal mismatch with slower chemical reaction dynamics substantially hinders its applicability. Herein, we demonstrate light-driven steady-state and on-demand catalyst spin modulation that effectively activates plasmonic catalysis. The rapidly oscillating plasmonic electromagnetic near-field spin-polarizes a low-spin CoFe2O4 catalyst and overcomes the photobleaching to produce stable high-spin states with astounding spin lifetimes >60 μs. The high-spin plasmonic catalyst effectively balances the tradeoff between spin polarization and carrier dynamics. For benchmark light-driven nitrate reduction catalysis, it achieves substantial photo-enhancement in ammonia production rate and selectivity as well as photocatalytic performance driven by sunlight, benefiting from polarization activation of nitrate reactant and preferential reaction pathway modulation. The highly generalized light-mediated strategy opens intriguing new avenues for on-demand and steady-state electronic spin engineering with profound implications for distinct disciplines.

影响因子：

15.7

分区情况：

一区