CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Shuyi He,Zheguan Lin,Jie Shi,Linyu Zhou,Qingyan Cui,Tiesen Li,Jiangyong Liu,Yuanyuan Yue
For traditional strategies to construct SO 2 and H 2 O co-resistant systems in low-temperature NH 3 selective catalytic reduction (NH 3 -SCR) catalysts, the primary challenge lies in mitigating the partial loss of redox activity at active sites. Herein, we present an approach to construct a protective system based on interface engineering principles, effectively safeguarding Cu active sites in ZnO/FeCu-SSZ-13 under SO 2 and H 2 O exposure. The core innovation stems from the creation of a strong interface effect originated from Zn-O-Al bonds formed between ZnO and the framework Al on the FeCu-SSZ-13 surface. This interface effect can regulate the electronic structure of Zn O bonds on ZnO component, producing abundant basic sites around the Cu active sites, enabling the preferential adsorption of SO 2 and its oxidation into ZnSO 4 , thereby virtually eliminating the redox ability loss of Cu active sites. As a result, ZnO/FeCu-SSZ-13 achieves exceptional low-temperature NH 3 -SCR performance, maintaining over 90 % NO x conversion even in the presence of SO 2 and H 2 O. Our work opens a new avenue for developing low-temperature NH 3 -SCR catalysts with desired SO 2 and H 2 O resistance, offering valuable insights for advancing catalytic performance in challenging reaction conditions.
研究领域:
催化
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环境化学
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材料科学
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表面工程
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化学反应工程
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DOI
高影响因子
CATALYSIS TODAY
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2020
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IF 5.825
Ye Ma,Shichao Han,Qinming Wu,Longfeng Zhu,Huimin Luan,Xiangju Meng,Feng-Shou Xiao
The metal-exchanged zeolites as catalysts have been widely applied in many catalytic reactions , but their syntheses are environmentally unfriendly due to the multiple steps such as ion-exchange for the formation of a large amount of wastes. Herein, we for the first time report a method for one-pot fabrication of metal-zeolite catalysts (M-SSZ-13, M-Beta, M-ZSM-5, and M-EU-1; M = Cu, Co, Ni) from a combination of solvent-free and sodium-free routes by mixing, grinding, and heating the raw materials of aluminosilicate gel, organic templates, and metal-amine complexes. As a typical example, Cu-SSZ-13 zeolite is successfully synthesized from heating the mixture of aluminosilicate gel, organic template, and Cu-amine complex. Catalytic tests in selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) show that the synthesized Cu-SSZ-13 zeolite before and after hydrothermal aging at 750 °C for 16 h are completely comparable with the commercial Cu-SSZ-13 zeolite from the conventional hydrothermal synthesis. Very interestingly, the method in this work has obvious advantages such as high yield, reduced pollutants, and simple process, which should be potentially important for practical applications of the metal-zeolites in the future.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
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IF 12.2
Lin Zheguan,Cao Wanying,Cui Qingyan,Li Tiesen,Bao Xiaojun,Fu Xianzhi,Yue Yuanyuan
Water-induced deactivation of catalysts
under low-temperature
and
high-humidity conditions remains a major challenge for the practical
application of NH 3 -selective catalytic reduction (NH 3 -SCR) technology. Herein, a dynamic Brønsted acid site
compensation strategy based on the heterolytic dissociation of H 2 O is proposed to improve the water tolerance of Cu-based chabazite
catalysts. Following this strategy, a Co-WO 3 /FeCu-SSZ-13
catalyst was rationally designed. Co doping effectively modulates
the d-band center of WO 3 , enabling heterolytic H 2 O dissociation and the in situ generation of hydroxyl
groups that act as Brønsted acid sites, thereby significantly
enhancing NH 3 adsorption and activation. Simultaneously,
preferential utilization of H 2 O for Brønsted acid
site compensation mitigates its competitive occupation of the intrinsic
metal active sites in FeCu-SSZ-13, preserving the NO oxidation pathway
under high-humidity conditions. Therefore, this synergistic regulation
of dynamic compensation of Brønsted acid sites and the release
of active metal sites enables Co-WO 3 /FeCu-SSZ-13 to achieve
a NO x conversion exceeding 90% at 165
° C in the presence of 20 vol % H 2 O. This work highlights
the dual role of H 2 O in simultaneously regulating the acid
and redox cycles, offering a general strategy for designing water-tolerant
NH 3 -SCR catalyst.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Peipei Zhou,Ting Wu,Zhen Sun,Yinuo Liu,Xinwei Chen,Meihua Zhu,Fei Zhang,Na Hu,Yuqin Li,Tian Gui,Xiangshu Chen,Hidetoshi Kita
Here, high-silica SSZ-13 membranes were prepared on macroporous supports by regulating sodium sources (NaOH, NaCl, Na 2 SO 4 and sodium-free) under fluoride and aluminum free gel. A pure phase and high gas permeation SSZ-13 membrane with oval-shaped crystals on the membrane surface was obtained by NaCl. It suggests that alkali metal sodium ion promoted crystal crystallization. The influence of Na 2 O (2NaCl)/SiO 2 ratio (from 0.025 to 0.2) on the crystallization process of zeolite membranes was investigated in detail by XRD , SEM and gas permeation tests. The content of NaCl hardly affected the structure of SSZ-13 but could affect the morphology and size of the crystals. The best membrane (NaCl/SiO 2 = 0.2) had a mixed CO 2 and N 2 gas permeance of 5.4 × 10 −7 mol/(m 2 s Pa) and 5.2 × 10 −8 mol/(m 2 s Pa), along with the CO 2 /CH 4 and N 2 /CH 4 selectivity of 155 and 12.3, respectively. The effects of pressure drop, temperature and feed concentration on membrane separation performance were explored. In addition, the obtained SSZ-13 membrane exhibited the hydrothermal stability in the humid N 2 /CH 4 mixture under 298K, indicating the application prospects in natural gas separation.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
FUEL
·
2026
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IF 7.5
Yang Gao,Yue Ma,Letong Yang,Xiaodong Wu,Rui Ran,Yanyang Yu,Duan Weng
Cu-SSZ-13, a Cu-exchanged zeolite, has been applied as a NO x selective catalytic reduction (SCR) catalyst for diesel aftertreatment, but improving its durability remains a challenge. To address this issue, a core–shell Cu-SSZ-13@SAPO-34 catalyst was prepared by a microwave-assisted hydrothermal method. The evolution of copper species and zeolite framework during high-temperature hydrothermal aging, potassium poisoning and sulfur poisoning, as well as the impacts on SCR performance, was explored. Cu 2+ ions detached by hydrothermal aging could migrate from the Cu-SSZ-13 core to the SAPO-34 shell and be reactivated, owing to the close interface contact between the zeolites. When exposed to chemical poisoning by K + and SO 2 , the SAPO-34 shell effectively shielded the Cu-SSZ-13 core. Thus, more active Cu 2+ ions could be preserved to maintain the SCR performance of the catalyst.
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xueqin Wang,Tiesen Li,Chan Wang,Qingyan Cui,Tinghai Wang,Xiaojun Bao,Yuanyuan Yue
Designing a cost-effective and fast fabrication Cu-SSZ-13 with improved selective catalytic reduction of NO by ammonia (NH 3 -SCR) performance remains an open question. Here we report that LaCe-SSZ-13 zeolites were synthesized from spent fluid catalytic cracking catalyst within 12 h. After ion-exchanging with CuSO 4 solution, the obtained LaCeCu-SSZ-13 catalysts exhibit significantly higher catalytic activity and hydrothermal stability than conventional Cu-SSZ-13. Various characterizations reveal that La and Ce modification not only facilitates the disperse of isolated Cu 2+ species, but also effectively mitigates dealumination and inhibits copper species aggregation after hydrothermal aging. In-situ diffuse reflection infrared Fourier transform spectrum analyses demonstrate that La and Ce modification can accelerate the adsorption capacity for NH 3 and NO x and promote the decomposition of NH 4 NO 3 intermediate species on the catalyst, benefiting the improvement of low-temperature activity. The combination of experiments and theoretical calculations further demonstrate that the most stable positions of La and Ce are on different eight-membered rings in SSZ-13, and then Cu 2+ ions tend to enter eight-membered rings to enhance the NH 3 adsorption capacity and decrease the H 2 O adsorption capacity, which results in higher low-temperature activity and hydrothermal stability than Cu-SSZ-13. Our work provides a feasible strategy for preparing the efficient rare-earth-modified Cu-zeolite based NH 3 -SCR catalyst for nitrogen oxide abatement.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Mingwei Cai,Heng Liu,Jiongcai Chen,Luxin Sun,Jiahao Wu,Zhiyin Chen,Zhenjing Han,Tingting Cui,Shiyang Zhang,Yonggang Min,Xiaohua Ma
A crucial problem in membrane-based gas separation is to fabricate membranes with excellent permeability, selectivity, and stability. Here, a high-performance carbon molecular sieves membrane of TR-CMS/SSZ-13 was successfully produced by pyrolyzing a thermally rearranged (TR) mixed matrix membrane (MMM) that obtained from a copolyimide precursor (6FDA/ODA/6FAP(3:2)) and SSZ-13 zeolite as filler at 450 °C. The effect of SSZ-13 zeolite content and structures of precursors on the transport behavior of derived CMS membranes was thoroughly studied. After TR process, the as formed polybenzoxazole (PBO) chain resulted in an enhanced rigidity, higher fractional free volume (0.15 vs 0.17), and a significantly increased (1898 times) BET surface area. Further enhancing the treatment temperature to 650 °C, the formed TR-CMS membranes exhibited a huge improved BET surface area from 228.2 to 639.3 m 2 /g, delivering a remarkable gas separation performance with H 2 permeability of 7089 Barrer and H 2 /CH 4 selectivity of 136. When doping with SSZ-13 till 15 wt%, the TR-CMS/SSZ-13–15 % showed an even higher H 2 (9726 Barrer) and CO 2 permeability (6932 Barrer), as well as H 2 /CH 4 (150 vs 136) and CO 2 /CH 4 (107 vs 57) selectivity than the pure TR-CMS, which surpassed the newest 2019 Robeson Upper bound. This can associate with the strong interaction between the modified SSZ-13 and the polymer matrix that prevent the collapse of the aromatic strand during the pyrolysis process, thereby create more ultra-micropore volume and concentration. Conclusively, pyrolyzing TR-MMM precursor is an effective way to form high-performance membranes with good potential for CO 2 separation and H 2 purification.
研究领域:
材料科学
·
化学工程
·
膜技术
·
气体分离
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产品关联
DOI
高影响因子
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