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Near-infrared-driven photoelectrocatalytic oxidation of urea on La-Ni-based perovskites
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-05-27 , DOI: 10.1016/j.cej.2022.137240
Ying Tao , Linglong Chen , Zhong Ma , Chi Zhang , Yang Zhang , Dieqing Zhang , Donglai Pan , Jiabao Wu , Guisheng Li

The solar-driven photoelectrocatalytic oxidation of urea is an efficient and costly way to produce hydrogen and purify wastewater synergistically. However, it is still a big challenge facing to the semiconductor-catalyst photoanode with high utilization of sunlight. Herein, we report a series of La-Ni-based Ruddlesden-Popper phases perovskite materials (Lan+1NinO3n+1, n = 1, 2 and 3) for photoelectrocatalytic oxidations of urea. Such La-Ni -based perovskite materials act simultaneously as a light-harvesting semiconductor and as the electrocatalyst for urea oxidation and all of Lan+1NinO3n+1 catalysts display a strong near-infrared (NIR) light absorption (≥ 800 nm). The La4Ni3O10 catalyst exhibits the best activity towards urea oxidation reaction (UOR) with an applied potential of 1.54 V vs. RHE at 1 mA cm-2, compared to that of 1.64 V and 1.56 V vs. RHE for La2NiO4 and La3Ni2O7, respectively, and 44.7 μmol cm-2h-1 of N2 generation rate under NIR light irradiation at the potential of 1.62 V vs. RHE, which is 2.5 times and 1.8 times of that for La2NiO4 and La3Ni2O7, respectively. The unique structure of La4Ni3O10 accelerates the separation and transport of electrons and holes, which is beneficial for the diffusion and adsorption of urea molecules in photoanode.



中文翻译:

La-Ni基钙钛矿上近红外驱动的尿素光电催化氧化

太阳能驱动的尿素光电催化氧化是一种高效且昂贵的协同生产氢气和净化废水的方法。然而,对于太阳光利用率高的半导体催化剂光阳极来说,这仍然是一个很大的挑战。在此,我们报告了一系列用于尿素光电催化氧化的 La-Ni 基 Ruddlesden-Popper 相钙钛矿材料(La n+1 Ni n O 3n+1,n = 1、2 和 3)。这种基于 La-Ni 的钙钛矿材料同时作为集光半导体和尿素氧化的电催化剂和所有的 La n+1 Ni n O 3n+1催化剂显示出强烈的近红外 (NIR) 光吸收 (≥ 800 nm)。La 4 Ni 3 O 10催化剂对尿素氧化反应 (UOR) 表现出最佳活性,在 1 mA cm -2下施加电位为 1.54 V vs. RHE ,而 La 的施加电位为 1.64 V 和 1.56 V vs. RHE 2 NiO 4和La 3 Ni 2 O 7分别为44.7 μmol cm -2 h -1在NIR光照射下的N 2生成速率在1.62 V vs.RHE分别是La 2 NiO 4和La 3 Ni 2 O 7的2.5倍和1.8倍。La 4 Ni 3 O 10的独特结构加速了电子和空穴的分离和传输,有利于尿素分子在光电阳极中的扩散和吸附。

更新日期:2022-05-27
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