ACS Applied Materials & Interfaces
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2023
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IF 9.5
Mengzhen Song,Jingru Han,Yingzhi Wang,Lungang Chen,YanYan Chen,Xiaoyuan Liao
Fe-based MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts due to their well-developed pores and accessible active sites. However, their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based MOF catalysts. In this work, we manipulated the structure of Fe-oxo nodes in MIL-88B(Fe) via a CuI species substitution method, affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved Fenton-like performance. It is found that the CuI serves as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results. A linear relationship was observed for the Fenton-like performance and the amount of CuI species for the catalysts. The corresponding value of the •OH formation is 2.17 eV for Cu-incorporated MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe) (2.69 eV). Meanwhile, the enriched CuI species suppress Fe species leaching during the catalytic reaction. The Fe-ion leakage of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly less than that of MIL-88B (2.00–3.02 mg/L). At the same time, H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%, which is almost 4.4 times that of pure MIL-88B(Fe). This work provides insights into the rational design of Fe-MOFs as promising Fenton-like catalysts for wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Yichuan Li,Xinyan Zhang,Mingxing Luan,Yuntong Zhao,Shibin Feng,Zhaosheng Yang,Bin Liu,Yongming Chai
Molecular sieve membranes are widely used in separation and catalysis due to their good chemical and thermal stability, resistance to contamination, long life, and easy modification. Although immobilized molecular sieve membranes combine catalytic reactivity with recycling separation properties, preparing high-performance TS-1 molecular sieve membrane catalysts is still challenging. In this study, the oriented aggregation of nanocrystals was used in constructing molecular sieve membrane catalysts. By interfering with the crystallization of TS-1, pre-crystal modification with cetyltrimethoxysilane was employed to change the crystal growth behavior. Thus, uniform and dense molecular sieve membranes were prepared through the modulated crystallization of TS-1. This method reduced the requirements of the carrier surface properties for the loading of the membrane layer to enable the construction of membrane layers on carriers of different materials and shapes. Using this method, the effective H 2 O 2 utilization and the epichlorohydrin yield of the micron-sized spherical film catalyst prepared with the inexpensive templating agent TPABr in the chloropropene epoxidation reaction reached 95.89% and 90.22%, respectively.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2024
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IF 4.8
Yuqing Ouyang,Ningning Du,Xiaoyun Xiong,Qingxun Hu,Hongman Sun,Tingting Li,Jie Zhong,Youhe Wang,Zifeng Yan
The combination of titanium silicalite-1 (TS-1) zeolite and H 2 O 2 oxidant provides an excellent alternative to many highly toxic and polluting olefin oxidation processes due to the by-product being water-only and without deep oxidation. However, the diffusion of bulky reactants and products suffers from the inherent micropores of conventional TS-1 zeolites. Herein, we designed a reticulated ordered macroporous carbon material with uniform and coherent mesopores, and successfully synthesized ordered hierarchical TS-1 zeolites containing intracrystalline macroporous-mesoporous-microporous by dry gel method. The fully interconnected intracrystalline macroporous-mesoporous-microporous hierarchical TS-1 improves the accessibility of the active site and the diffusion efficiency of bulky compounds. It showed excellent catalytic performance during the epoxidation reaction of chloropropene, and its epichlorohydrin yield and H 2 O 2 effective utilization were 70.11% and 77.05%, which were 2.2 and 1.9 times of the catalytic performance of commercial TS-1 zeolites, respectively, and significantly better than the ultrafine TS-1 synthesized by conventional methods. The high catalytic performance was maintained after three cycles of use. This offers a good opportunity for the design and synthesis of efficient zeolite catalysts in the future.
研究领域:
材料科学
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化学工程
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催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AIR & WASTE MANAGEMENT ASSOCIATION
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2016
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IF 1.613
Jiade Wang,Binxun Hong,Xinyang Tong,Shufeng Qiu
The process of recovering waste sulfuric acids using H2O2 catalytic oxidation is studied in this paper. Activated carbon was used as catalyst. Main operating parameters, such as temperature, feed rate of H2O2, and catalyst dosage, have effects on the removal of impurities from waste sulfuric acids. The reaction kinetics of H2O2 catalytic oxidation on impurities are discussed. At a temperature of 90°C, H2O2 feeding rate of 50 g (kg waste acid)−1 per hour, and catalyst dosage of 0.2 wt% (waste acid weight), the removal efficiencies of COD and chrominance were both more than 99%, the recovery ratio of sulfuric acid was more than 95%, and the utilization ratio of H2O2 was 88.57%.Implications: Waste sulfuric acid is a big environmental problem in China. The amount of waste sulfuric acid is huge every year. Many small and medium-sized businesses produced lots of waste acids, but they don’t have an appropriate method to treat and recover them. H2O2 catalytic oxidation has been used to treat and recover waste sulfuric acid and activated carbon is the catalyst here. Main parameters, such as temperature, feed rate of H2O2, and catalyst dosage, have been investigated. The reaction kinetics are discussed. This method can be economical and feasible for most small and medium-sized businesses.
研究领域:
环境科学
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化学工程
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废物处理
✓ 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）