
近日,暨南大学朱明山团队报道了基于细胞色素c的半人工光酶一步深度氧化NO过程中抑制NO2生成。相关论文于2026年2月23日发表在《德国应用化学》杂志上。
太阳能驱动催化在分子氧活化和低浓度氮氧化物消除方面具有潜力,但实现NO高选择性转化为无毒硝酸盐(NO3-)同时抑制有毒NO2生成仍具挑战。
研究组报道了一种通过将单血红素细胞色素c(cyt c)固定在氮化碳(CN)上构建的半人工光酶催化剂,通过精细化调控活性物种实现NO深度氧化。该杂化光酶催化剂在cyt c与CN界面构筑局域内建电场(IEF),促进激子解离的同时,在cyt c表面形成优先吸附O2的极化活性位点,通过电子转移途径将O2活化为活性过氧化物(•O2-和*O22-),并抑制1O2生成。
在cyt c/CN催化剂上,NO一步氧化为NO3-的反应得到显著促进,展现出优异的催化性能:在空速(WHSV)为850 L·g-1·h-1的宽湿度范围内,NO转化率达97.4%,NO2选择性极低(1.5%,6.5 ppb),且具有长期稳定性(300 min后仍保持98.1%)。其有害副产物NO2生成量显著低于纯CN(17.0%,104.7 ppb)及文献报道的催化剂。该催化剂在直接去除NO2(92.9%)方面也表现出高活性,并在模拟环境舱中能将NO浓度快速降至安全浓度(52 ppb)以下。
附:英文原文
Title: Suppression of NO2 Generation During One-Step Deep Oxidation of NO at a Semi-Artificial Photoenzyme Based on Cytochrome c
Author: Jing Wang, Jingling Yang, Jialin Li, Tianle Cai, Mingshan Zhu
Issue&Volume: 2026-02-23
Abstract: Solar-driven catalysis holds promise in molecular oxygen activation and low-concentration NOx elimination but achieving highly selective conversion of NO to nontoxic nitrate (NO3), while suppressing toxic NO2 formation remains challenging. Here, we report a semi-artificial photoenzyme catalyst constructed by immobilizing mono-heme cytochrome c (cyt c) on carbon nitride (CN) to refine reactive species generation for deep NO oxidation. The hybrid photoenzyme catalyst establishes localized internal electric fields (IEF) between cyt c and CN that promote exciton dissociation, and creates polarized active sites on cyt c that preferentially adsorb O2, and activate O2 to active peroxides (O2 and *O22) via an electron transfer pathway with inhibiting 1O2 formation. The one-step NO oxidation to NO3 is boosted over cyt c/CN, showing exceptional 97.4% NO conversion with ultralow NO2 selectivity (1.5%, 6.5 ppb) and long-term stability (98.1% after 300 min) at a weight hourly space velocity (WHSV) of 850 L g1·h1 across wide humidity ranges. The undesirable NO2 generation is significantly lower than that of bare CN (17.0%, 104.7 ppb) and reported catalysts. The catalyst exhibits high activity in direct NO2 removal (92.9%) and rapidly reduces NO levels to below the safe concentration (52 ppb) in a simulated environment chamber.
DOI: 10.1002/anie.3296119
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.3296119
Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx
