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使用铑改性的二氧化钛光催化剂通过水合肼的完全分解实现可见光辅助制氢。

Visible light assisted hydrogen generation from complete decomposition of hydrous hydrazine using rhodium modified TiO photocatalysts.

作者信息

Kumar Pawan, Kumar Anurag, Queffélec Clémence, Gudat Dietrich, Wang Qi, Jain Suman L, Boukherroub Rabah, Szunerits Sabine

机构信息

Chemical Sciences Division, CSIR-Indian Institute of Petroleum, Dehradun-248005, India.

Chimie Et Interdisciplinarité: Synthèse Analyse Modélisation (CEISAM), Université de Nantes, CNRS, UMR 6230, 2, rue de la Houssinière, BP 92208, 44322 Nantes Cedex 3, France.

出版信息

Photochem Photobiol Sci. 2017 Jul 1;16(7):1036-1042. doi: 10.1039/c6pp00432f. Epub 2017 May 26.

Abstract

Hydrogen is considered to be an ideal energy carrier, which produces only water when combined with oxygen and thus has no detrimental effect on the environment. While the catalytic decomposition of hydrous hydrazine for the production of hydrogen is well explored, little is known about its photocatalytic decomposition. The present paper describes a highly efficient photochemical methodology for the production of hydrogen through the decomposition of aqueous hydrazine using titanium dioxide nanoparticles modified with a Rh(i) coordinated catechol phosphane ligand (TiO-Rh) as a photocatalyst under visible light irradiation. After 12 h of visible light irradiation, the hydrogen yield was 413 μmol g cat with a hydrogen evolution rate of 34.4 μmol g cat h. Unmodified TiO nanoparticles offered a hydrogen yield of 83 μmol g cat and a hydrogen evolution rate of only 6.9 μmol g cat h. The developed photocatalyst was robust under the experimental conditions and could be efficiently reused for five subsequent runs without any significant change in its activity. The higher stability of the photocatalyst is attributed to the covalent attachment of the Rh complex, whereas the higher activity is believed to be due to the synergistic mechanism that resulted in better electron transfer from the Rh complex to the conduction band of TiO.

摘要

氢气被认为是一种理想的能量载体,它与氧气结合时仅产生水,因此对环境没有有害影响。虽然用于制氢的水合肼催化分解已得到充分研究,但其光催化分解却鲜为人知。本文描述了一种高效的光化学方法,即在可见光照射下,以用Rh(I)配位儿茶酚膦配体修饰的二氧化钛纳米颗粒(TiO-Rh)作为光催化剂,通过水合肼水溶液的分解来制氢。可见光照射12小时后,产氢量为413 μmol g催化剂,析氢速率为34.4 μmol g催化剂 h。未改性的TiO纳米颗粒的产氢量为83 μmol g催化剂,析氢速率仅为6.9 μmol g催化剂 h。所开发的光催化剂在实验条件下具有稳定性,并且可以有效地重复使用五次,其活性没有任何显著变化。光催化剂较高的稳定性归因于Rh配合物的共价连接,而较高的活性据信是由于协同机制,该机制导致从Rh配合物到TiO导带的电子转移更好。

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