APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xiao Yu,Mengyi Shi,Yixuan Fan,Lixia Yang,Jie Zhang,Wei Liu,Weili Dai,Shuqu Zhang,Lei Zhou,Xubiao Luo,Shenglian Luo
Mn 2 O 3 is an exceptional earth-abundant mineral that has been extensively applied in catalytic oxidation because of the strong redox couples like Mn 3+ /Mn 2+ and Mn 4+ /Mn 3+ exposed on Mn 2 O 3 surface. Herein, the catalytic activity of Mn 2 O 3 in photothermal degradation of toluene was regulated by halogens including F - , Cl -, and Br - . As the electronegativity ordered in F (3.98) > O (3.44) > Cl (3.16) > Br (2.96), F - doped Mn 2 O 3 overperforms Cl - doped and Br - doped Mn 2 O 3 in decomposing toluene. DFT theoretical calculation illustrates that F - attracts the shared electrons from Mn to itself, the deviated charge center stretches the adjacent Mn-O bonds and boosts the generation of abundant oxygen vacancies, helping to strengthen the catalytic activity of Mn 2 O 3 . Conversely, Mn-O bonds are shortened by Cl - and Br - that have lower electronegativity than O. The multiple electrons circling Cl - and Br - push Mn towards O and squeeze Mn-O bonds, resulting in the formation of passivated Mn 2 O 3 . In conjunction with Mn redox couples and oxygen vacancies, 99% of 400 ppm toluene can be eliminated by F - doped Mn 2 O 3 , corresponding mineralization rate is high up to 95.8%.
研究领域:
催化
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环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiahui Jiang,Bingbing Gong,Guancheng Xu,Ting Zhao,Hui Ding,Yuying Feng,Yixuan Li,Li Zhang
CeO 2 has been identified as a significant cocatalyst to enhance the electrocatalytic activity of transition metal phosphides (TMPs). However, the electrocatalytic mechanism by which CeO 2 enhances the catalytic activity of TMP remains unclear. In this study, we have successfully developed a unique CeO 2 -CoP-1–4 multishell microsphere heterostructure catalyst through a simple hydrothermal and calcination process. CeO 2 -CoP-1–4 exhibits great potential for electrocatalytic oxygen evolution reaction (OER), requiring only an overpotential of 254 mV to achieve a current density of 10 mA cm −2 . Moreover, CeO 2 -CoP-1–4 demonstrates excellent operating durability lasting for 55 h. The presence of CeO 2 as a cocatalyst can regulate the microsphere structure of CoP, the resulting multishell microsphere structure can shorten the mass transfer distance, and improve the utilization rate of the active site. Furthermore, in situ Raman and ex situ characterizations, and DFT theoretical calculation results reveal that CeO 2 can effectively regulates the electronic structure of Co species, reduces the reaction free energy of rate-limiting step, thus increase the reaction kinetic. Overall, this study provides experimental and theoretical evidence to better comprehend the mechanism and structure evolution of CeO 2 in enhancing the OER performance of CoP, offering a unique design inspiration for the development of efficient hollow heterojunction electrocatalysts.
研究领域:
材料科学
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电化学
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催化
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
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2022
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IF 8.943
Hui Su,Xudan Dou,Dandan Xu,Li Feng,Yongze Liu,Ziwen Du,Liqiu Zhang
The massive use of personal medicines makes them widely enter the aquatic environments and cause pollution, drawing a great deal of attention over the last few years. In this study, a novel nano Fe 0 -loaded superfine powdered activated carbon (Fe 0 @SPAC) was prepared via a simple ball milling method. Fe 0 @SPAC showed a rapid and effective removal for aqueous carbamazepine (CBZ) via the process of synergistic adsorption and persulfate (PDS) activation. The removal efficiency of CBZ (30 mg L −1 ) could be up to 96% by Fe 0 @SPAC (0.05 g L −1 ) with the presence of PDS (2 mM), and the maximum pseudo-first-order rate constant was 0.12 min −1 . The performance of Fe 0 @SPAC was superior to other reported iron-bearing activator materials, and its dosage was much lower. Fe 0 @SPAC was also effective to remove other typical drug pollutants and had excellent reusability in five cycles. The loaded Fe 0 could activate PDS to generate OH and SO 4 − , which played the major role for CBZ removal. It is interesting that carbon base of Fe 0 @SPAC could also activate PDS via surface defects , making the minor contribution to CBZ degradation. Besides, Fe 0 @SPAC showed rapid and high adsorption for CBZ due to the superfine particle diameter, partially contributing to CBZ removal. Finally, the possible break sites of CBZ and its degradation pathway were proposed based on DFT theoretical calculation and product identification. Fe 0 @SPAC would be a promising material for the removal of drug pollutants, and this study may help understand the mechanisms of synergistic adsorption and persulfate activation by carbon composite material.
研究领域:
环境科学
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水处理
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）