The production of hydrogen and benzaldehyde (BAD) by splitting benzyl alcohol (BA) through photocatalysts is one of the common methods of converting solar energy to chemical energy. Herein, a photocatalyst to achieve high efficiency in hydrogen production was fabricated by loading Cu-Ni bi-metal on the CdS nanorods as a carrier. The 20% Cu 1 Ni 1 /CdS composite catalyst was used for simultaneous photocatalyze H 2 production and BA oxidation to BAD under light with activities of 14.517 and 13.220 mmol g -1 h −1 , respectively, which is 8.7 times and 7.9 times higher than that of pure CdS . The high production efficiency can be mainly attributed to the synergistic effect of Cu-Ni bi-metal and the close contact between Cu-Ni and CdS interfaces. These microstructures enhance light absorption, effectively promote charge separation, and reduce the complexation of photogenerated electrons and holes. This work provides new ideas for the design of a cost-effective catalyst.
Zhe Liu,Qi Liu,Xuhua Zhang,BingRui Shi,Dandan Qin,Jiaxuan Wang,Aining Zhang,Yongjun Liu
In this study, the sewage sludge was converted into sludge biochar (SBC) and doped with Cu-Ni bimetal to synthesize a novel composite catalyst (Cu-Ni@SBC) for the activation of H 2 O 2 for phenol degradation. Characterization results showed that the Cu-Ni bimetal was successfully doped into the SBC and led to the formation of a porous structure with abundant cavities, resulting in a larger specific surface area and higher adsorbed oxygen content. Mechanism analysis revealed a valence state conversion cycle between Cu 0 -Cu(II), Ni(III)-Ni(II) and Cu-Ni which made Cu-Ni@SBC have higher electron transfer performance. Response surface methodology was applied to determine the optimal preparation and reaction conditions, under which the Fenton-like system composed of Cu-Ni@SBC and H 2 O 2 removed 100 % of phenol and mineralized 69.1 % of TOC from simulated wastewater. In addition, the experimental results showed that the Cu-Ni@SBC material had a relatively wide pH adaptation range (4–8), and the removal efficiency of phenol could reach 76.4 % after 5 cycles of experiments, and the catalytic inhibition rates of the two common coexisting anions, HCO 3 – and Cl - , were 17.1 % and 0 %, respectively. The results of practical application revealed that the phenol removal efficiency reached 90.44 % and the pollutant mineralization rate could reach 58.5 % within 90 min, which proved that the catalyst was suitable for the advanced degradation of organic matter in coal chemical wastewater. Therefore, Cu-Ni@SBC can be considered as a promising Fenton-like catalyst, and the process method is also of some guiding significance for the treatment of coal chemical wastewater.
Hu Changjiang,Jiang Zhiwen,Wu Qunyan,Cao Shuiyan,Li Qiuhao,Chen Chong,Yuan Liyong,Wang Yunlong,Yang Wenyun,Yang Jinbo,Peng Jing,Shi Weiqun,Zhai Maolin,Mostafavi Mehran,Ma Jun
The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO 2 and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CH 3 OH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min −1 ) with a cost-effective hydroxyl radical scavenger promotes CH 3 OH production rate to 0.27 mmol g −1 min −1 . Moreover, time-resolved experiments with calculations reveal the direct generation of CO 2 •‒ radical anions via aqueous electrons attachment occurred on nanosecond timescale, and cascade hydrogenation steps. Our study highlights a radiolytic route to produce CH 3 OH with CO 2 feedstock and introduces a desirable atomic structure to improve performance.