Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide
Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide
复制标题
氮化碳上原子分散的锑用于过氧化氢的人工光合作用
DOI：
10.1038/s41929-021-00605-1
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发表时间：
2021-05-01
期刊：
影响因子：
37.8
通讯作者：
Ohno, Teruhisa
中科院分区：
文献类型：
--
作者：
Teng, Zhenyuan;Zhang, Qitao;Ohno, Teruhisa
人工光合作用为生产过氧化氢（H₂O₂）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，光催化过程中两电子氧还原反应（ORR）的低活性和选择性极大地限制了H₂O₂的生产效率。在此，我们展示了一种性能强大的锑单原子光催化剂（Sb - SAPC，单锑原子分散在氮化碳上），它能在可见光照射下于简单的水和氧气混合物中合成H₂O₂。实现了在420 nm处17.6%的表观量子产率以及H₂O₂合成0.61%的太阳能 - 化学转化效率。基于含时密度泛函理论计算、同位素实验和先进的光谱表征，光催化性能归因于通过在锑位点形成μ - 过氧化物以及在相邻氮原子处高度聚集的空穴，显著促进了两电子氧还原反应。通过水氧化原位生成的O₂被氧还原反应迅速消耗，从而提高了整体反应动力学。过氧化氢是人工光合作用一个有趣的目标，尽管通过两电子氧还原反应实际生产它仍然受限。现在，一种氮化碳负载的锑单原子光催化剂已被开发出来，在此过程中具有优异性能。
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 mu-peroxide at the Sb sites and highly concentrated holes at the neighbouring N atoms. The in situ generated O-2 via water oxidation is rapidly consumed by ORR, leading to boosted overall reaction kinetics.Hydrogen peroxide is an interesting target for artificial photosynthesis, although its actual production via the two-electron oxygen reduction reaction remains limited. Now, a carbon nitride-supported antimony single atom photocatalyst has been developed with a superior performance for this process.