Photocatalytic coproduction of H2 and industrial chemical over MOF-derived direct Z-scheme heterostructure
Photocatalytic coproduction of H2 and industrial chemical over MOF-derived direct Z-scheme heterostructure
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DOI：
10.1016/j.apcatb.2020.119066
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发表时间：
2020-09-15
影响因子：
22.1
通讯作者：
Lu, Tong-Bu
中科院分区：
文献类型：
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作者：
Liu, Meng;Qiao, Li-Zhen;Lu, Tong-Bu
人工光合作用同时产生氢-2和有价值的化学品是非常可取的，作为一种有希望的整体水分裂的替代方案。在本文中，通过对多元金属有机骨架硫化过程中均匀分布的金属阳离子的自识别，构建了Z-方案Co9S8/CDS异质结构。原位生成的CdS和Co9S8形成直接的Z型异质结，有利于界面电荷的分离，氧化和还原电位分别达到2.09V和-0.74V(vs.RHE)。对于苯甲醇(BA)在纯水中的高选择性氧化，其析氢活性高达61,924 mU·mol·g~(-1)，分别是单独的硫化镉和Co9S8/硫化镉物理混合物的21倍和16倍。这项工作为从固体溶液中构建Z-方案异质结构提供了一种新的策略，从而大大提高了H-2燃料和有价值的化学品的联合生产，而不需要任何牺牲剂。
Artificial photosynthesis for simultaneously producing H-2 and valuable chemicals is extremely desirable to act as a promising alternative for overall water splitting. Herein, a Z-scheme Co9S8/CdS heterostructure was constructed by self-recognition of uniformly distributed metal cations during the sulfidation of a multivariate metal-organic framework. The intimate contact of in situ formed CdS and Co9S8 into direct Z-scheme heterostructure can facilitate interfacial charge separation and extend the oxidation and reduction potentials to 2.09 V and -0.74 V (vs. RHE), respectively. An excellent H-2 evolution activity of 61,924 mu mol g(-1) with high selectivity for benzyl-alcohol (BA) oxidation in pure water is achieved, ca. 21 and 16 times higher than that of isolated CdS and physical mixture of Co9S8/CdS. This work supplies a new strategy for constructing Z-scheme heterostructure from a solid solution to dramatically boost coproduction of H-2 fuel and valuable chemicals without any sacrificial agents.