NH2-MIL-125(Ti) with transient metal centers via novel electron transfer routes for enhancing photocatalytic NO removal and H2 evolution

NH2-MIL-125(Ti) with transient metal centers via novel electron transfer routes for enhancing photocatalytic NO removal and H2 evolution
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DOI:
10.1039/d1cy01008e
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发表时间:
2021-07-27
影响因子:
5
通讯作者:
He, Youzhou
He, Youzhou
中科院分区:
化学2区
文献类型:
--
作者:
Li, Houfan;Liu, Xingyan;He, Youzhou

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通过简便的方法合成的双功能光催化剂Yb-NH2-MIL-125(Ti)增强了光催化脱除NO和产氢的同时,其中锚定在NH2-MIL-125(Ti)上的Yb种瞬态中心的形成加快了载流子的转移和分离速度。最优样品Yb-NM-6的NO去除率为66.3%(原NH2-MIL-125(Ti)仅为28.1%),产氢量为1883.7993 μ mol g(-1)(原NH2-MIL-125(Ti)几乎没有影响)。一系列对比实验,特别是循环伏安测试表明,通过非传统的配体-连接体金属电荷转移(LLMCT)途径获得瞬态Yb-II/III中心,与传统的配体-金属电荷转移(LMCT)途径有很大不同,从而形成新的电荷转移通道,提高光催化性能。这项工作详细介绍了一种可行的途径,通过引入锚定在金属有机框架上的各种金属离子作为有效的瞬态中心,进一步提高光催化性能,从而获得一种新的LLMCT途径。
The bifunctional photocatalyst Yb-NH2-MIL-125(Ti) synthesized using a simple and convenient method enhanced photocatalytic NO removal and hydrogen production simultaneously, in which the formation of Yb species transient centers anchored on NH2-MIL-125(Ti) accelerated the transfer and separation rate of charge carriers. The NO removal rate of the optimal sample Yb-NM-6 was 66.3% (the original NH2-MIL-125(Ti) was only 28.1%), and the hydrogen production was 1883.7993 mu mol g(-1) (the original NH2-MIL-125(Ti) had almost no effect). A series of comparative experiments, in particular cyclic voltammogram tests, showed that the transient Yb-II/III centers were obtained through a non-traditional ligand to linker metal charge transfer (LLMCT) pathway, which was very different from the traditional ligand metal charge transfer (LMCT) pathway, so as to form a novel charge transfer channel to improve photocatalytic performance. This work details a feasible avenue by which to obtain a novel LLMCT pathway through introducing various metal ions anchored on metal-organic frameworks as efficient transient centers to further improve photocatalytic performance.