Qichao Chen,Chengjie Lu,Boyu Ping,Guiyang Li,Jiayi Chen,ZhengMing Sun,Yuanjian Zhang,Qiushi Ruan,Li Tao
Scalable solar-driven H 2 O 2 evolution from water holds great promise for industrial applications. Efficient H 2 O 2 generation relies on excellent spatial charge separation but simultaneously suffers from severe surface H 2 O 2 backreaction, which becomes a bottleneck for scalable H 2 O 2 evolution. Herein, a hydroxyl-induced carbon nitride (CN) homojunction coherently optimizes the bulk charge separation and suppresses surface backreaction. Surface hydroxyls provide extra electron accommodation bands for electron extraction from the bulk to the surface which are visually observed with KPFM and rationalized by DFT calculations. 2e - oxygen reduction reaction (ORR) kinetic became more favorable than 4e - ORR in the presence of hydroxyl, showing suppressed H 2 O 2 decomposition. This homojunction achieves a 4.5-fold improvement in H 2 O 2 production compared to pristine CN, and an apparent quantum yield (AQY) of 2.1 % at 500 nm in water. This work demonstrates a strategy for coherently improving spatial charge separation and surface reaction kinetics, which is applicable for various photocatalytic reactions.
The complex reaction interface and the high reaction barrier for C─C coupling hinder the conversion of CO 2 toward high-value C 2+ products. In this work, thiol is employed to modify facet-controlled Cu nanoparticles, systematically elucidating the tripartite interaction between organic modifiers, active sites, and key intermediates. Theoretical calculations, Kelvin Probe Force Microscope (KPFM), and in situ investigations reveal that the thiol-derived spatial potential field facilitates CO 2 activation and the formation of hydrocarbon intermediates ( * COH). More importantly, the results demonstrate that the C 2+ products of the thiol-modified catalyst are strongly dependent on the crystal planes: the potential field preferentially drives suitable adsorbed * COH to asymmetric * CO- * COH coupling on Cu (100)/(111) interface. Consequently, the C 2+ selectivity of the thiol-modified Cu (100)/(111) interface-rich Cu nanoparticle is intrinsically enhanced, exhibiting high selectivity to C 2+ products with a faradaic efficiency (FE) of 85.44%. Remarkably, the structure achieves a C 2 H 4 FE of 73.79% ± 2.69% with a peak partial current density of 345.75 mA cm − 2 (total current: 1.38 A). Beyond establishing a high-efficiency CO 2 to C 2+ conversion protocol, this study provides mechanistic insights into the selective steering of C─C coupling through tailored surface modifications.
危险品化学品经营许可证（带存储）