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ACS Omega · 2023 · IF 4.1

Preparation of Micron-Sized TS-1 Spherical Membrane Catalysts and Their Performance in the Epoxidation of Chloropropene

Guoqiang Tang,Yichuan Li,Zhaosheng Yang,Yu Wang,Guangyun Li,Yilou Wang,Yong-Ming Chai,Chenguang Liu

Titanium silica (TS-1) membrane catalysts grown on the surfaces of spherical substrates can both exploit the high catalytic performance and facilitate their separation from products after the reaction. In this work, a simple static crystallization method was used to perform the in situ construction of a TS-1 membrane on the surfaces of micron-sized spherical carriers. The shortcomings of the TS-1 membrane under static crystallization conditions were overcome by in situ dynamic crystallization, and the effect of rotation speed on the formation of the molecular sieve membrane was investigated. The results showed that the molecular sieve membrane was smooth and homogeneous, with a higher synthesis efficiency at a slow rotational speed. The micron TS-1 spherical membrane catalytic chloropropene epoxidation reaction was investigated in a fixed bed, and the conversion of hydrogen peroxide and selectivity of epichlorohydrin reached 99.4 and 96.8%, respectively. After being reused twice, the catalyst still maintained a stable catalytic performance.

研究领域: 化学工程 · 催化材料科学
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ACS Applied Materials & Interfaces · 2020 · IF 8.758

BaTiO3 Nanosheets and Caps Grown on TiO2 Nanorod Arrays as Thin-Film Catalysts for Piezocatalytic Applications

Enzhu Lin,Ni Qin,Jiang Wu,Baowei Yuan,Zihan Kang,Dinghua Bao

Powder-form piezocatalysts suffer from poor recyclability and pose a potential threat of creating serious secondary pollution, which restrict their practical applications. Thin-film piezocatalysts, which not only exhibit good recyclability but also fully contact with solution, are believed to be one of the solutions to address these problems. In this work, the nanostructured BaTiO3 (BTO) thin films were fabricated by a facile hydrothermal method for their potential applications in piezocatalysis. The vertically standing BTO nanosheets grown on the top of TiO2 nanorod arrays exhibited superior piezocatalytic performance as well as piezo-electrochemical property. Given the different strain states between thin-film piezocatalyst and powder-form piezocatalyst, both the impact force of water and isostatic pressure are taken into consideration in finite element method (FEM) simulation. The FEM simulation shows that a stronger piezoelectric filed can be built in BTO nanosheets because of their easier deformation, and thus can lead to a higher piezocatalytic degradation efficiency. Our work presented here is expected to provide a potential route for the nanoengineering of thin-film piezocatalysts and clarify the catalytic mechanism for substrate-fixed piezocatalysts.

研究领域: 材料科学 · 环境科学 · 催化化学
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 23 ·11051-11062 · IF 3.3

Preparation of a microfibrous Fe/LTA zeolite membrane catalyst for acetone oxidation: effect of the preparation method

Chengzhi Hu,Changyan Zhou,Huiping Zhang,Ying Yan

Chemical vapor deposition (CVD) and impregnation (IM) methods were applied in the preparation of novel Fe/LTA (Linde Type A) zeolite membrane/paper-like sintered stainless steel fiber (Fe/LTA/PSSF) catalysts for acetone oxidation. The catalysts were characterized using various techniques, such as actual iron loading (AAS), surface morphology (SEM), phase composition and crystallite size (XRD), specific surface area (BET), valence state (XPS) and reducibility (H2-TPR), to investigate the effects of the calcination process, iron loading, preparation methods and supports on their catalytic activity. The calcined catalysts were more active than the non-calcined catalysts in the catalytic oxidation of acetone due to the different oxidation states of the deposited metal species. The catalysts prepared by CVD with an Fe loading of 2.29% exhibited similar activity to the IM-prepared catalysts with Fe loadings of 4.42% and 9.69%, which may be attributed to the superior dispersion of the active Fe2O3 phases, the smaller size of metal oxide and the increased ability for oxygen storage. Among the IM-prepared catalysts, Fe/LTA/PSSF-IM-2 with an Fe loading of 4.42% exhibited the lowest T90 of 230 °C. Additionally, the catalysts coated on LTA/PSSF showed higher activity and contact efficiency (T90 of 249 °C) compared to those on granular zeolite (T90 of 318 °C).

研究领域: 催化化学 · 环境科学
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Construction of immobilized spherical TS-1 molecular sieve membranes using oriented aggregation of nanocrystals

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 · 催化材料科学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Facile Preparation of Hydrogen-Bonded Organic Framework/Cu2O Heterostructure Films via Electrophoretic Deposition for Efficient CO2 Photoreduction

An-An Zhang,Yu-Lin Li,Zhi-Bin Fang,Lei Xie,Rong Cao,Yangyang Liu,Tian-Fu Liu

Photocatalytic CO2 reduction is one of the most cost-effective and environmentally friendly techniques of converting CO2 into high-value compounds and/or fuels. However, the performance of most current photocatalytic CO2 reduction catalysts is less than satisfactory for practical applications. Here, we synthesized a heterogeneous structure by integrating Cu2O and a porphyrin hydrogen-bonded organic framework (PFC-45), which was then fabricated into a thin-film catalyst on carbolic paper (CP) using a facile electrophoretic deposition technology. With improved electron–hole separation efficiency and visible-light-harvesting ability, this film (PFC-45/Cu2O@CP) significantly enhanced CO2-to-CO photoreduction, exceeding 2.4 and 3.2 times that of PFC-45@CP and PFC-45/Cu2O particles, respectively. Remarkably, PFC-45/Cu2O@CP also exhibited high selectivity (99%) and outstanding activity (11.81 μmol g–1 h–1) for photocatalytic CO2 reduction in pure water without any sacrificial agent. This work demonstrates a new strategy to design photocatalysts for efficient CO2 reduction.

CAS / MDL: 142439-89-2
研究领域: 材料科学 · 环境科学 · 化学工程 · 光化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-13 · IF 14.7

Main-group element-boosted oxygen electrocatalysis of Cu-N-C sites for zinc-air battery with cycling over 5000 h

Li Yifan,Huang Aijian,Zhou Lingxi,Li Bohan,Zheng Muyun,Zhuang Zewen,Chen Chang,Chen Chen,Kang Feiyu,Lv Ruitao

Developing highly active and durable air cathode catalysts is crucial yet challenging for rechargeable zinc-air batteries. Herein, a size-adjustable, flexible, and self-standing carbon membrane catalyst encapsulating adjacent Cu/Na dual-atom sites is prepared using a solution blow spinning technique combined with a pyrolysis strategy. The intrinsic activity of the Cu-N 4 site is boosted by the neighboring Na-containing functional group, which enhances O 2 adsorption and optimizes the rate-determining step of O 2 activation (*O 2  → *OOH) during the oxygen reduction reaction process. Meanwhile, the Cu-N 4 sites are encapsulated within carbon nanofibers and anchored by the carbon matrix to form a C 2 -Cu-N 4 configuration, thereby reinforcing the stability of the Cu centers. Moreover, the introduction of Na-containing functional groups on the carbon atoms significantly reduces the positive charge on their outer shell C atoms, rendering the carbon skeletons less susceptible to corrosion by oxygen species and further preventing the dissolution of Cu centers. Under these multi-type regulations, the zinc-air battery with Cu/Na-carbon membrane catalyst as the air cathode demonstrates long-term discharge/charge cycle stability of over 5000 h. This considerable stability improvement represents a critical step towards developing Cu-N 4 active sites modified with the neighboring main-group metal-containing functional groups to overcome the durability barriers of zinc-air batteries for future practical applications.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 电化学 · 能源存储
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