光催化
材料科学
石墨氮化碳
掺杂剂
载流子
离解(化学)
活动站点
氮化硼
化学键
光化学
氮化碳
纳米技术
兴奋剂
化学
催化作用
物理化学
有机化学
光电子学
作者
Mahmoud Kamal Hussien,Amr Sabbah,Mohammad Qorbani,P. Raghunath,Septia Kholimatussadiah,Der‐Lii M. Tzou,Mohamed Hammad Elsayed,Yu Lu,Yen‐Yu Wang,Xing‐Hao Lee,Ting-Yun Lin,Nguyȇñ Quȏć Thãńg,Heng‐Liang Wu,Shu‐Chih Haw,Kevin C.‐W. Wu,Ming‐Chang Lin,Kuei‐Hsien Chen,Li‐Chyong Chen
出处
期刊:Small
[Wiley]
日期:2024-04-19
标识
DOI:10.1002/smll.202400724
摘要
Abstract The lack of intrinsic active sites for photocatalytic CO 2 reduction reaction (CO 2 RR) and fast recombination rate of charge carriers are the main obstacles to achieving high photocatalytic activity. In this work, a novel phosphorus and boron binary‐doped graphitic carbon nitride, highly porous material that exhibits powerful photocatalytic CO 2 reduction activity, specifically toward selective CO generation, is disclosed. The coexistence of Lewis‐acidic and Lewis‐basic sites plays a key role in tuning the electronic structure, promoting charge distribution, extending light‐harvesting ability, and promoting dissociation of excitons into active carriers. Porosity and dual dopants create local chemical environments that activate the pyridinic nitrogen atom between the phosphorus and boron atoms on the exposed surface, enabling it to function as an active site for CO 2 RR. The P–N–B triad is found to lower the activation barrier for reduction of CO 2 by stabilizing the COOH reaction intermediate and altering the rate‐determining step. As a result, CO yield increased to 22.45 µmol g −1 h −1 under visible light irradiation, which is ≈12 times larger than that of pristine graphitic carbon nitride. This study provides insights into the mechanism of charge carrier dynamics and active site determination, contributing to the understanding of the photocatalytic CO 2 RR mechanism.
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