Pb-Activated Amine-Assisted Photocatalytic Hydrogen Evolution Reaction on Organic–Inorganic Perovskites

产品简述

期刊

JACS


标题

Pb-Activated Amine-Assisted Photocatalytic Hydrogen Evolution Reaction on Organic–Inorganic Perovskites


作者

Lu Wang, Hai Xiao , Tao Cheng , Youyong Li, William A. Goddard

摘要

We report here the reaction mechanism for explicit aqueous solvent quantum mechanics (QM) studies determining the energetics and reaction barriers for the photocatalytic hydrogen evolution reaction (HER) on CH3NH3PbI3 surface. We find that both the lead (Pb) atoms and the surface organic molecules play essential roles, leading to a two-step Pb-activated amine-assisted (PbAAA) reaction mechanism involving an intermediate lead hydride state. Both H of H2 product are extracted from surface organic molecules, while two protons from the solution migrate along water chains via the Grotthuss mechanism to replace the H in organic molecule. We obtain a reaction barrier of 1.08 eV for photochemical generation of H2 on CH3NH3PbI3 compared to 2.61 eV for the dark reaction. We expect this HER mechanism can also apply to the other organic perovskites, but the energy barriers and reaction rates may depend on the basicity of electrolyte and intrinsic structures of perovskites.


原文链接

https://pubs.acs.org/doi/10.1021/jacs.7b12028


2018年03月16日

添加时间:

Mesoscale Graphene-like Honeycomb Mono- and Multilayers Constructed via Self-Assembly of Coclusters

上一个:

下一个:

Core–Shell ZIF-8@ZIF-67-Derived CoP Nanoparticle-Embedded N-Doped Carbon Nanotube Hollow Polyhedron for Efficient Overall Water Splitting
  • 1