Nonmetal Atom Doping Induced Orbital Shifts and Charge Modulation at the Edge of Two-Dimensional Boron Carbonitride Leading to Enhanced Photocatalytic Nitrogen Reduction

Abstract

Electronic structure, particularly charge state analysis, plays a crucial role in comprehending catalytic mechanisms. This study focuses on metal-free boron carbonitride (BCN) nanosheets as a case study to investigate the impact of heteroatom doping on the charge state of active sites at the edge of two-dimensional (2D) metal-free nanomaterials. Our observations revealed that the doping induces a shift in the frontier p y orbital near the Fermi level, accompanied by alterations in its charge state. These changes provide insights into the nitrogen adsorption descriptors and the critical hydrogenation step, ultimately leading to the proposal of a competitive charge transfer mechanism. Additionally, this exploration has led to the screening of five BCN-type structures (

Theoretical Prediction and Synthesis of Nonmetal-Doped Anatase TiO2 (101) for Boosting Photocatalytic Hydrogen Evolution Reaction

“…Photocatalysis is a promising technology for the production of clean energy using sunlight-excited semiconductor photocatalysts. − Hydrogen is the world’s cleanest energy source. − The high density and low pollution characteristics of hydrogen energy have made hydrogen evolution and application technologies a focus of attention in the 21st century. In the background of global energy demand and the global carbon cycle, researchers have explored a large number of photocatalysts for hydrogen evolution. − However, most photocatalysts are prone to photogenerated carrier recombination under light excitation, , resulting in inadequate photocatalytic efficiency.…”

Flatland materials for photochemical and electrochemical nitrogen fixation applications: from lab-door experiments to large-scale applicability

“…12–15 The efficiency of the photochemical and electrochemical nitrogen reduction reaction (NRR) for NH 3 production relies upon the prudent choice of a catalytic system that can accelerate the reaction dynamics. 16–21 A wide array of catalytic systems has been constructed by researchers to augment the yield of the targeted renewable energy carrier during energy-conversion applications. These systems include perovskites, 22,23 mesoporous materials, 24,25 transition metal oxides 26 /phosphides 27 /dichalchogenides 28 /carbonitrides/borides, 29,30 single-atom catalysts (SACs), 31,32 layered double hydroxides (LDHs), 33,34 and carbon-based derivatives.…”