过电位
质子耦合电子转移
电子转移
质子
水溶液
化学物理
Pourbaix图
分解水
化学
电子
催化作用
材料科学
光化学
电化学
物理化学
电极
物理
光催化
有机化学
量子力学
作者
Jun Cheng,Xiandong Liu,John A. Kattirtzi,Joost VandeVondele,Michiel Sprik
标识
DOI:10.1002/anie.201405648
摘要
Abstract The high overpotential in water oxidation on anodes is a limiting factor for the large‐scale application of photoelectrochemical cells. To overcome this limitation, it is essential to understand the four proton‐coupled electron transfer (PCET) steps in the reaction mechanism and their implications to the overpotential. Herein, a simple scheme to compute the energies of the PCET steps in water oxidation on the aqueous TiO 2 surface using a hybrid density functional is described. An energy level diagram for fully decoupled electron‐ and proton‐transfer reactions in which both electronic and protonic levels are placed on the same potential scale is also described. The level diagram helps to visualize the electronic and protonic components of the overpotential, and points out what are needed to improve. For TiO 2 , it is found that its catalytic activity is due to aligning the protonic energy levels in the PCET steps, while improving the activity requires also aligning the electronic levels.
科研通智能强力驱动
Strongly Powered by AbleSci AI