Li Bo, Zheng Hongshun, Zhou Tong, Lu Qingjie, Chen Mingpeng, Sun Huachuan, Zhang Yuxiao, Zhang Yumin, Li Dequan, Zi Baoye, Zhang Mao, Zhang Jin, Zhao Jianhong, He Tianwei, Zhu Zhongqi, Zhang Genlin, Liu Qingju
Yunnan Key Laboratory for Micro/Nano Materials & Technology, National Center for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming, 650091, China.
Southwest United Graduate School, Kunming, 650091, PR China.
Nat Commun. 2025 Sep 12;16(1):8276. doi: 10.1038/s41467-025-63637-2.
Integrating distinct functional reaction sites within a single photocatalyst offers a promising approach for enhancing the photocatalytic H evolution by water splitting. However, the synergy between the dual active sites is hindered by suboptimal electronic states arising from the uniform coordination environments. Here we demonstrate a strategy for enhancing the synergy between Pt single atoms and nanoparticles by modulating the coordination environment. The optimal boron doped catalyst with B-Pt-O asymmetric coordination achieves a H evolution rate of 627.6 mmol gh, with an apparent quantum efficiency of 98.4%. Experimental and theoretical analysis reveal that the asymmetric coordination structure redistributes the electron density of Pt cocatalysts, promoting charge carrier separation, optimizing the dissociation and adsorption-desorption of the intermediate HO* and H* on the dual sites. The findings highlight the importance of asymmetric coordination facilitates the photogenerated carrier transfer and surface reactions for efficient photocatalytic H evolution.
在单一光催化剂中整合不同的功能反应位点为通过水分解增强光催化析氢提供了一种有前景的方法。然而，由于均匀配位环境产生的次优电子态阻碍了双活性位点之间的协同作用。在此，我们展示了一种通过调节配位环境来增强铂单原子与纳米颗粒之间协同作用的策略。具有B-Pt-O不对称配位的最佳硼掺杂催化剂实现了627.6 mmol g h的析氢速率，表观量子效率为98.4%。实验和理论分析表明，不对称配位结构重新分布了铂助催化剂的电子密度，促进了电荷载流子的分离，优化了中间体HO和H在双位点上的解离以及吸附-解吸。这些发现突出了不对称配位对于促进光生载流子转移和表面反应以实现高效光催化析氢的重要性。
