Dispersive XAFS Study on the Laser-Induced Reduction of a Rh3+ Ion Complex: Presence of a Rh+ Intermediate in Direct Photoreduction
Dispersive XAFS Study on the Laser-Induced Reduction of a Rh3+ Ion Complex: Presence of a Rh+ Intermediate in Direct Photoreduction
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Rh3 离子络合物激光诱导还原的色散 XAFS 研究：直接光还原中 Rh 中间体的存在
DOI：
10.1021/acs.jpcc.1c10160
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Ohba Hironori
中科院分区：
文献类型：
--
作者：
Saeki Morihisa;Matsumura Daiju;Nakanishi Ryuzo;Yomogida Takumi;Tsuji Takuya;Saitoh Hiroyuki;Ohba Hironori
采用色散x射线吸收精细结构光谱学研究了脉冲紫外激光诱导Rh3+离子配合物直接光还原成rh0的反应机理。时间分辨x射线吸收近边结构（XANES）显示没有等吸点，表明有两种以上的Rhn+参与了Rh3+的直接光还原。奇异值沉积法分析时间分辨XANES数据表明，直接光还原涉及三种Rhn+。对时间分辨XANES数据进行交替最小二乘分析，得到三种Rhn+的纯光谱和浓度分布曲线。根据XANES纯光谱特征，将Rhn+归属于Rh3+、Rh+和rh0种。浓度曲线表明，直接光还原的顺序为Rh3+→Rh+→Rh0。提出了Rh3+和Rh+的光还原、Rh3+和Rh+的光诱导自催化还原和Rh+的光氧化反应机理，可以很好地再现3种Rhn+的浓度分布。
The reaction mechanism of the direct photoreduction of a Rh3+ion complex to a Rh0species induced by pulsed ultraviolet laser irradiation was studied using dispersive X-ray absorption fine structure spectroscopy. The time-resolved X-ray absorption near edge structure (XANES) showed the absence of isosbestic points and suggested that more than two Rhn+species contribute toward the direct photoreduction of Rh3+. Analysis of the time-resolved XANES data by singular value deposition showed that the direct photoreduction involves three Rhn+species. Multivariate curve resolution by alternating least-squares analysis of the time-resolved XANES data gave pure spectra and the concentration profiles of the three Rhn+species. The Rhn+species were assigned to Rh3+, Rh+, and Rh0species based on the features of the pure XANES spectra. The concentration profiles suggested that the direct photoreduction proceeds in the order of Rh3+→ Rh+→ Rh0. A reaction mechanism, which was proposed involving photoreductions of Rh3+and Rh+, photoinduced autocatalytic reductions of Rh3+and Rh+, and photooxidation of Rh+, well reproduced the concentration profiles of three Rhn+species.
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