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正交 WP 共催化剂与电子转移桥 UiO-66 耦合,用于高效可见光驱动的 H 演化。

Orthorhombic WP co-catalyst coupled with electron transfer bridge UiO-66 for efficient visible-light-driven H evolution.

机构信息

School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, PR China; Ningxia Key Laboratory of Solar Chemical Conversion Technology, North Minzu University, Yinchuan 750021, PR China; Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, PR China.

School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan 750021, PR China; Ningxia Key Laboratory of Solar Chemical Conversion Technology, North Minzu University, Yinchuan 750021, PR China; Key Laboratory for Chemical Engineering and Technology, State Ethnic Affairs Commission, North Minzu University, Yinchuan 750021, PR China.

出版信息

J Colloid Interface Sci. 2019 Nov 15;556:689-703. doi: 10.1016/j.jcis.2019.08.107. Epub 2019 Aug 29.

DOI:10.1016/j.jcis.2019.08.107
PMID:31499440
Abstract

The abundant transition metal phosphides co-catalysts on the earth can satisfy the sustainable and clean solar H production through photocatalytic water splitting, which is promising to replace the rare precious metals, such as Pt, Au, Pd, Ru and so on. In this paper, we use the temperature-programmed solid phase method to prepare WP nanoparticles. Based on the Density Functional Theory (DFT) calculations, we demonstrate that the WP nanoparticles possess outstanding electrical conductivity and excellent capability to transport electrons. WP nanoparticles are loaded onto the surface of UiO-66 via the ultrasound-assisted impregnation method to induce a highly efficient visible-light photocatalytic H production activity of 384 µmol in 5 h, which is 10.67 times than that of pure UiO-66. The catalytic performance is attributed to the excellent metallic conductivity and the favourable Fermi level position of WP nanoparticles. Further studies of PL, TRPL and Mott-Schottky curves, we can not only know that the modification of WP nanoparticles do improve the electron transfer ability, but also that the matched work functions between the EY and UiO-66 provides a feasible thermodynamic path for the transmission of electrons. Our work demonstrates that the earth-abundant transition metal phosphides material have the potential to construct cheaper and high catalytic performance photocatalysts.

摘要

丰富的过渡金属磷化物共催化剂在地球上可以通过光催化水分解来满足可持续和清洁的太阳能 H 生产,有望取代稀有贵金属,如 Pt、Au、Pd、Ru 等。本文采用程序升温固相法制备 WP 纳米粒子。基于密度泛函理论(DFT)计算,我们证明 WP 纳米粒子具有出色的导电性和优异的电子传输能力。通过超声辅助浸渍法将 WP 纳米粒子负载到 UiO-66 表面,诱导出高效的可见光光催化 H 生产活性,在 5 小时内产生 384 µmol 的 H2,是纯 UiO-66 的 10.67 倍。这种催化性能归因于 WP 纳米粒子的优异金属导电性和合适的费米能级位置。进一步的 PL、TRPL 和 Mott-Schottky 曲线研究表明,WP 纳米粒子的修饰不仅可以提高电子转移能力,而且 EY 和 UiO-66 之间的功函数匹配为电子传输提供了可行的热力学途径。我们的工作表明,丰富的过渡金属磷化物材料有可能构建更廉价和高催化性能的光催化剂。

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