CO2 photoreduction into highly value-added chemicals over metal-free h-BCN has emerged as a promising strategy to address the issue of global warming. However, the serious carrier recombination caused by disordered charger transfer has limited its practical application. To circumvent this issue, fluorine modified h-BCN were synthesized using a facile heat treatment method. The surface halogenation created local spatial polarized electric field, which facilitated the local charge separation and transmission efficiency. Among them, BCN-F-4 exhibited the best photocatalytic CO2 reduction activitiy with CO and CH4 yield of 25.38 and 14.11 µmol g−1h−1, respectively. The turnover number (TON) of BCN-F-4 reached up to 163.6 μmol g−1h−1, 4.4 times that of BCN. Both theoretical simulation and experimental analysis demonstrated a strong covalent interaction between the F atoms and the h-BCN matrix, which gain deep understanding of the mechanism of prominent photocatalytic CO2 reduction activity boosted by surface halogenation.

中文翻译：

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氟化硼碳氮化物中的局部空间极化诱导有效电子转移以促进 CO2 光还原


通过无金属 h-BCN 将二氧化碳光还原成高附加值化学品已成为解决全球变暖问题的一项有前景的策略。然而，无序电荷转移引起的严重载流子复合限制了其实际应用。为了解决这个问题，使用简单的热处理方法合成了氟改性的 h-BCN。表面卤化产生局部空间极化电场，有利于局部电荷分离和传输效率。其中，BCN-F-4表现出最好的光催化CO2还原活性，CO和CH4产率分别为25.38和14.11 µmol g−1h−1。 BCN-F-4的周转数（TON）达到163.6 μmol g−1h−1，是BCN的4.4倍。理论模拟和实验分析都证明了F原子和h-BCN基质之间存在很强的共价相互作用，这使得人们对表面卤化增强光催化CO2还原活性的机制有了深入的了解。