Xiao Jiangrong, Chen Shengtao, Jin Jingpeng, Li Renjie, Zhang Jing, Peng Tianyou
College of Urban Construction, Wuchang Shouyi University, Wuhan 430070, China.
College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China.
Langmuir. 2021 Oct 26;37(42):12487-12500. doi: 10.1021/acs.langmuir.1c02282. Epub 2021 Oct 14.
The solar-driven CO reduction reaction (CORR) for producing chemical fuels is considered to be a promising approach to dealing with the growing energy crisis and greenhouse effect. Herein, novel Ag/MnO dual-cocatalyst-decorated brookite titania (BT) nanoparticles with remarkably boosted photocatalytic CORR performance are prepared through a facile photodeposition method. The resultant Ag-BT-Mn composite with optimal cocatalyst content delivers amazing CO/CH yields of 31.70/129.98 μmol g with an overall photoactivity of 1103.28 μmol g h, 11.98 times higher than that of the BT nanoparticles alone. Further investigations demonstrate that the dual cocatalysts decorating the BT nanoparticles not only effectively retard the photoinduced charge recombination but also significantly vary the surface chemical feature to promote the adsorption/activation of the reactants (CO/HO). In addition, the Ag nanoparticles can broaden the spectral response region, while the MnO cocatalyst can promote the CH product selectivity and the water oxidation reaction. The synergistic effect of Ag/MnO dual cocatalysts on the BT nanoparticles renders a remarkably boosted CORR performance, which provides a simple yet general synthesis strategy for brookite titania-based photocatalysts with high-performance solar-driven CO conversion.
利用太阳能驱动的一氧化碳还原反应(CORR)来生产化学燃料,被认为是应对日益严重的能源危机和温室效应的一种很有前景的方法。在此,通过一种简便的光沉积方法,制备了具有显著增强的光催化CORR性能的新型双助催化剂修饰的板钛矿型二氧化钛(BT)纳米颗粒。具有最佳助催化剂含量的所得Ag-BT-Mn复合材料实现了31.70/129.98 μmol g的惊人CO/CH产量,总光活性为1103.28 μmol g h,比单独的BT纳米颗粒高出11.98倍。进一步的研究表明,修饰在BT纳米颗粒上的双助催化剂不仅有效地抑制了光生电荷复合,而且显著改变了表面化学特性,以促进反应物(CO/H₂O)的吸附/活化。此外,Ag纳米颗粒可以拓宽光谱响应区域,而MnO助催化剂可以提高CH产物的选择性和水氧化反应。Ag/MnO双助催化剂在BT纳米颗粒上的协同作用使得CORR性能显著提高,这为基于板钛矿型二氧化钛的高性能太阳能驱动CO转化光催化剂提供了一种简单而通用的合成策略。