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Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide
Nature Catalysis ( IF 37.8 ) Pub Date : 2021-05-21 , DOI: 10.1038/s41929-021-00605-1
Zhenyuan Teng , Qitao Zhang , Hongbin Yang , Kosaku Kato , Wenjuan Yang , Ying-Rui Lu , Sixiao Liu , Chengyin Wang , Akira Yamakata , Chenliang Su , Bin Liu , Teruhisa Ohno

Artificial photosynthesis offers a promising strategy to produce hydrogen peroxide (H2O2)—an environmentally friendly oxidant and a clean fuel. However, the low activity and selectivity of the two-electron oxygen reduction reaction (ORR) in the photocatalytic process greatly restricts the H2O2 production efficiency. Here we show a robust antimony single-atom photocatalyst (Sb-SAPC, single Sb atoms dispersed on carbon nitride) for the synthesis of H2O2 in a simple water and oxygen mixture under visible light irradiation. An apparent quantum yield of 17.6% at 420 nm together with a solar-to-chemical conversion efficiency of 0.61% for H2O2 synthesis was achieved. On the basis of time-dependent density function theory calculations, isotopic experiments and advanced spectroscopic characterizations, the photocatalytic performance is ascribed to the notably promoted two-electron ORR by forming μ-peroxide at the Sb sites and highly concentrated holes at the neighbouring N atoms. The in situ generated O2 via water oxidation is rapidly consumed by ORR, leading to boosted overall reaction kinetics.



中文翻译:

氮化碳上原子分散锑用于过氧化氢的人工光合作用

人工光合作用为生产过氧化氢 (H 2 O 2 ) 提供了一种有前景的策略——过氧化氢是一种环境友好型氧化剂和清洁燃料。然而,光催化过程中双电子氧还原反应(ORR)的低活性和选择性极大地限制了H 2 O 2的生产效率。在这里,我们展示了一种稳健的锑单原子光催化剂(Sb-SAPC,分散在氮化碳上的单个 Sb 原子),用于在可见光照射下在简单的水和氧气混合物中合成 H 2 O 2 。H 2 O 2在 420 nm 处的表观量子产率为 17.6%,太阳能化学转化效率为 0.61%实现了合成。基于时间相关的密度函数理论计算、同位素实验和先进的光谱表征,光催化性能归因于通过在 Sb 位点形成μ-过氧化物和在相邻 N 原子上形成高度集中的空穴来显着促进双电子 ORR . 通过水氧化原位产生的 O 2被 ORR 迅速消耗,从而提高了整体反应动力学。

更新日期:2021-05-21
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