For aqueous interfacial reactions involving H+and OH-, the interfacial pH varies dynamically during the reaction process, which is a key factor determining the reaction performance. Herein, the kinetic relevance betwe...For aqueous interfacial reactions involving H+and OH-, the interfacial pH varies dynamically during the reaction process, which is a key factor determining the reaction performance. Herein, the kinetic relevance between the interfacial pH and reaction rate is deciphered owing to the success in establishing the transport equations of H+/OH- in unbuffered solutions, and is charted as a current(j)–pH diagram in the form of an electrochemical response. The as-described j–pH interplay is experimentally verified by the oxygen reduction and hydrogen evolution reactions. This diagram serves to form a panoramic graphic view of pH function working on the interfacial reactions in conjunction with the Pourbaix’s potential–pH diagram, and particularly enables a kinetic understanding of the transport effect of H+and OH-on the reaction rate and valuable instruction toward associated pH control and buffering manipulation.展开更多
基金the National Natural Science Foundation of China(51525805,51727812,51808526)。
文摘For aqueous interfacial reactions involving H+and OH-, the interfacial pH varies dynamically during the reaction process, which is a key factor determining the reaction performance. Herein, the kinetic relevance between the interfacial pH and reaction rate is deciphered owing to the success in establishing the transport equations of H+/OH- in unbuffered solutions, and is charted as a current(j)–pH diagram in the form of an electrochemical response. The as-described j–pH interplay is experimentally verified by the oxygen reduction and hydrogen evolution reactions. This diagram serves to form a panoramic graphic view of pH function working on the interfacial reactions in conjunction with the Pourbaix’s potential–pH diagram, and particularly enables a kinetic understanding of the transport effect of H+and OH-on the reaction rate and valuable instruction toward associated pH control and buffering manipulation.