FUEL PROCESSING TECHNOLOGY
·
2023
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IF 7.5
Yu Tang,Yi Cui,Gaosheng Ren,Ke Ma,Xiaoxun Ma,Chengyi Dai,Chunshan Song
In this study, the copper-mordenite zeolite (Cu-MOR) and non-thermal plasma were used to produce methanol and hydrogen from methane and water at low temperature (120 °C) without CO 2 formation. Energy efficiency for methanol and hydrogen were 68.8 mmol·kJ −1 and 562.3 mmol·kJ −1 , respectively, and the selectivity of methanol in liquid products reached 86%. The reaction mechanism likely involves methane being excited to methyl (·CH 3 ) and hydrogen radicals (·H) under DBD plasma conditions, which can then adsorb on the catalyst surface at the Cu 2 -(μ-O) 2+ active sites, accompanied by water co-adsorption to facilitate formation and desorption of methanol. XPS analysis showed that with the prolongation of reaction time, Cu 2 -(μ-O) 2+ was reduced to Cu + and Cu(II) hydroxide, and the catalyst had carbon deposition , resulting in the decrease of catalytic activity . It is also worth noting that in an oxygen atmosphere, Cu 2 -(μ-O) 2+ regenerates rapidly and eliminates catalyst carbon deposits . Trace oxygen was introduced into the reactor, and the reaction was carried out for 30 h, and the catalytic activity did not decrease.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
GREEN CHEMISTRY
·
2025
·Vol. 27
·期 6
·1838-1857
·
IF 9.2
Li Yang,Bonan Liu,Yingying Zhao,Zijian Zhang,Hanyu Wu,Minyi He,Chao Tang,Jun Zhao,Yu Fan,Wangjing Ma
Modern chemists dream of a low-temperature bioethanol dehydration to ethylene process promoted by biomaterial-based catalysts, which would be without doubt an energy-saving, sustainable achievement in green chemistry. However, limitations on catalytic activity and competition from exothermic side reactions have always been an insurmountable gap. Herein, a microwave-assisted pathway employing biochar-based catalysts was designed to effectively dehydrate ethanol into ethylene at temperatures lower than 100 °C. Either biochar (BC) or phosphoric acid-modified derivate (HBC) was synthesized from bamboo powder through a simple one-step decomposition. ZSM-5/MOR composite zeolite was further introduced to form HBC-2-ZSM-5/MOR hybrid catalysts, which could effectively prevent the formation of diethyl-ether and enhance the production of ethylene. With a microwave input power and reaction temperature as low as 10 W and 82 °C, ethanol (WHSV = 2 h−1) could be completely converted on the HBC-2-ZSM-5/MOR (1.5) catalyst with almost 100% ethylene selectivity. Similar results were obtained in the conversion of bioethanol (model), Chinese liquor and beer, pointing to the wide applicability of this strategy. Investigation of the potential mechanism found that weak acidity, special structure and P-modification characteristics can effectively inhibit the formation of diethyl ether by-products, oligomerization and the coking process, which is conducive to promoting the selective conversion of ethanol to ethylene. This work has blazed another trail for low-temperature ethanol to ethylene by combining the advantage of microwave heating with precise tailoring of biochar-based catalysts, all for a better future life with green chemistry.
研究领域:
绿色化学
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催化材料科学
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DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2022
·Vol. 96
·期 12
·2747-2756
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IF 0.791
Li Xixi,Lu Xinhuan,Jing Run,Zhang Haifu,Wang Chenlong,Zhang Huaxin,Wang Beibei,Zhou Dan,Xia Qinghua
Abstract The MOR supported cobalt complex materials were synthesized by ion exchange method and used to catalyze the epoxidation reaction of α-pinene with air. The liquid phase batch mode of epoxidation reaction was carried out under atmospheric pressure and aerobic conditions. Among the supported [Co(NH 3 ) 6 ] 3+ -zeolites catalysts, [Co(NH 3 ) 6 ] 3+ -MOR exhibited the best catalytic efficiency for the titled reaction, and high reaction conversion as well as epoxidation product selectivity were obtained for α-pinene and α-epoxypinane. Parametric studies were performed to examine the effect factors like the Co content, the solvent, the initiator, the substrate amount and the catalyst amount. The catalyst can be reused at least nine cycles without significant loss in activity towards epoxidation.
研究领域:
化学工程
·
催化材料
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Linkai Wang,Yu Han,Jian Wei,Qingjie Ge,Shijian Lu,Yanpeng Mao,Jian Sun
Hydrogenation of CO 2 into light olefins is an important route to carbon neutrality . Most of traditional researches focus on the catalyst component, structure, and promoter to enhance the selectivity of light olefins while ignoring the diffusion of products. Here, we report a NaFeZr-MOR composite catalyst for light olefin synthesis in CO 2 hydrogenation via pore confinement. The selectivity in hydrocarbons and STY (Space-time yields) of C 2–4 = is gradually increasing maximum up to 51.3% and 12.2 (mmol·g cat −1 . h −1 ), which lie in a high level among reported Fe-based catalysts. Further characterization revealed that the essence of selectivity change period is the accumulation and evolution of carbonaceous species, which causes the change of product diffusion behavior. It suppresses the escape of heavy hydrocarbons from MOR pores, leading to an increased light olefin, especially ethylene, which is called “dynamic confinement”. These findings provide a new insight for controlling low-carbon product selectivity in CO 2 hydrogenation.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhipeng Qie,Minghui Hu,Wenqi He,Yao Zhang,Zhongbao Liu,Huaizhong Xiang,Zepeng Wang,Dafeng Yang,Shuyi Yao,Xinxin Pi,Hongxing Dai
Capturing CO 2 from humid flue gas remains a major challenge due to the severe competitive adsorption between CO 2 and H 2 O on zeolites. In this study, a novel chelation-assisted K + ion exchange strategy was proposed to simultaneously enhance both the CO 2 adsorption capacity and moisture resistance of mordenite (MOR) zeolites. Compared to the conventional ion exchange, this approach induced the mild surface dealumination, effectively removed the hydrophilic extra-framework Al(VI), and increased the K + exchange content. Structural refinement revealed that in the resulting MOR-EDTA-2K sample, K + ions were distributed in both the 12-membered ring (12MR) channels and the 8MR side pockets, which favored CO 2 adsorption. MOR-EDTA-2K achieved comparable uptake of 15 vol% CO 2 (46 mg/g) but with lower H 2 O uptake than conventional ion-exchange derived MOR sample, resulting in an improved CO 2 /H 2 O selectivity. Furthermore, DRIFTS analysis confirmed a mechanistic shift in CO 2 adsorption status from the HCO 3 − to CO 3 2− species, attributed to the inhibited water adsorption on MOR-EDTA-2K. For practical application, monolithic adsorbents prepared with MOR-EDTA-2K demonstrated prolonged CO 2 breakthrough time, excellent cyclic stability, and well regeneration at 75 °C. This facile and scalable method, with the advantage of low-temperature regeneration, renders the prepared zeolite a highly promising candidate for industrial CO 2 capture under humid conditions.
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Ting Zhang,Juan Huang,Yongbin Yang,Chunmei Li,Jianfeng Tang,Qing Li,Hua Lin
The development of bifunctional non-noble metal electrocatalysts with high activity and stability remains a significant challenge. In this work, Fe@Ni aerogels with core-shell structure were synthesized by sol-gel method. The unique network-like architecture and amorphous core-shell structures of Fe@Ni aerogels provide abundant defects and unsaturated sites. Moreover, the tunable surface electronic structure enhances the availability of active catalytic sites, resulting in outstanding catalytic performance for both the oxygen evolution reaction (OER) and methanol oxidation reaction (MOR). For OER, the FeNi 2 aerogel requires only an overpotential of 215 mV to achieve a current density of 10 mA cm −2 , along with a low Tafel slope of 31.7 mV dec −1 and excellent stability. For MOR, its specific and mass activities were as high as 213.6 mA cm −2 and 106.8 A g −1 , respectively. In addition, this study also elucidated the mechanism of the excellent bifunctional catalytic activity of Fe@Ni core-shell aerogels, which provides a new idea for the development of other high-activity non-precious metal electrocatalysts.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 7
·1066
·
IF 3.9
Xi’an Guan,Yehong Wang,Xiumei Liu,Hong Du,Xinwen Guo,Zongchao Zhang
As clean energy, methane has huge reserves and great development potential in the future. Copper zeolites are efficient in the oxidation of methane to methanol. Water has been confirmed as a source of oxygen to regenerate the copper-zeolite active sites to enable selective anaerobic oxidation of methane to methanol. In this work, we report that the methanol yield increased from 36 μmol/g (Cu-MOR1) to 92 μmol/g (Cu-MOR1-water) as a result of water enhancing the activity of copper ion-exchange mordenite catalyst. We show for the first time that water could convert inactive copper species into active copper species during catalyst activation. A combination of the XPS, FTIR, and NMR results indicates that water dissociates and then converts ZCuIIZ into ZCuII(OH) (where Z indicates framework O (Ofw) bonded to one isolated Al in a framework T-site, i.e., 1Al) and simultaneously produces a Brönsted acid site during catalyst activation. This finding can be used to tune the state of copper species and design highly active copper-zeolite catalysts for methane oxidation to methanol.Keywords:Cu-MOR;water;methane to methanol;ZCuIIOH;XPS
研究领域:
催化
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化学工程
·
材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Feng Chen,Xiao-Bo Feng,Jing-Ping Zhao,Zi-Meng He,Li-Yun Zhang,Yu-Hui Wang,Pan Deng,Xin-Hua Gao,Xiao-Yan Zhao,Jing-Pei Cao
Mordenite (MOR) zeolite is an efficient catalyst for dimethyl ether (DME) carbonylation, which a key step of indirect production of ethanol from syngas. Herein, a nanosheets MOR zeolite with an ultrathin thickness of 10–30 nm can be facilely synthesized by using a commercial cetyltrimethylammonium hydroxide agent. It greatly shortened the pore length of 8-membered ring (8-MR) side pocket and more amount of Brønsted acid sites (BAS) can be exposed. More importantly, the amount of BAS in 8-MR side pockets of the MOR zeolite can be significantly increased. It should be noted that the morphology of MOR zeolite with prismatic, nanosheets, and petal-like can be obtained and precisely regulated. As a result, the conversion of DME over the nanosheets MOR zeolite is increased by nearly 2 times. Our finding proposed a novel strategy for constructing tunable nanosized morphology MOR zeolite and simultaneously directional enrichment of BAS in 8-MR channels.
研究领域:
化学工程
·
材料科学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2026
·
IF 5.8
Yun Hu,Wei Wang,Fang Han,Zhicheng Wang,Qingqing Guo,Tianyu Chen,Fei-Yan Yi
The oxygen evolution reaction (OER) remains a major bottleneck in electrochemical water splitting due to its sluggish kinetics and high overpotential. Replacing the OER with thermodynamically more favorable oxidation reactions, such as the urea oxidation reaction (UOR) and methanol oxidation reaction (MOR), offers a promising strategy to reduce energy consumption while enabling value-added chemical production or wastewater treatment. In this work, a hydrangea-like trimetallic FeCoNi nanoalloy grown on nickel foam (FeCoNi/NF) and its nanosulfide (S–FeCoNi/NF) are developed as a unified electrocatalytic platform for OER, UOR, and MOR. The S–FeCoNi/NF electrode exhibits significantly enhanced performance, achieving an overpotential of 196 mV for OER and low operating potentials of 1.348 and 1.325 V for UOR and MOR, respectively, at 10 mA cm–2, surpassing the undoped FeCoNi/NF, outperforming most of the reported electrocatalysts. Experimental results reveal that sulfur doping effectively modulates the electronic structure, increases active site availability, and accelerates the reaction kinetics. This work highlights the potential of ternary transition metal sulfides as multifunctional electrocatalysts for energy-saving hydrogen production coupled to organic oxidation.
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DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 4
·854
·
IF 3.1
Peixuan Lin,Song Ye,Ling Pan,Ruihao Huang,Haoran Zhang,Deping Wang
In this research, upconversion nanocrystals incorporated with MOR zeolite composites were synthesized using the desilicated MOR zeolite as a host for the in situ growth of NaREF4(RE = Y, Gd) Yb/Er nanocrystals. The structure and morphology of the composites were studied with XRD, XPS, and TEM measurements, and the spectral studies indicated that the subsequent thermal treatment can effectively improve the upconversion emission intensity of Er3+. By using the NaYF4:Yb/[email protected]composite that holds the strongest upconversion emission, a probe of UCNC@DSiMOR/BPEI was constructed with the modification of branched poly ethylenimine for the detection of Cu2+. It was indicated that the integrated emission intensity of Er3+shows a linear dependence with the logarithm value of the Cu2+concentration ranging from 0.1 to 10 μM. This study offered a feasible method for the construction of UCNC@zeolite composites with enhanced upconversion emission, which may have a potential application as fluorescent probes for the detection of various metal ions by adjusting the doping luminescent center.
研究领域:
材料科学
·
分析化学
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DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Yumeng Xia,Zehua Li,Ying Li,Kai Cai,Yunduo Liu,Jing Lv,Shouying Huang,Xinbin Ma
Dimethyl ether (DME) carbonylation is an important reaction for methyl acetate (MA) and ethanol production from syngas. Mordenite (MOR) has been used as an industrial catalyst due to the competitive catalytic properties, especially with extremely high selectivity of MA (>99%). Given the Brønsted acid sites (BAS) in 8-MR are proved the active centers, the properties of BAS are crucial factors that influence the reaction. Until now, most of the researches focus on increasing the number of BAS rather than tuning the acid strength. Here we modified H-MOR by Ga introduction using incipient wetness impregnation. Catalyst evaluation results suggest that Ga species can enhance DME conversion with a maintained MA selectivity. Combining with characterizations and DFT calculation, the textural and acidic properties along with the existing form of Ga species are determined. Further in-situ IR, theoretical and kinetics investigations demonstrated that the enhanced acid strength accelerates the reaction on Ga-modified MOR catalysts. This work inspires us that improving the acid strength is an efficient strategy for Brønsted acid-catalyzed reaction, such as DME carbonylation .
研究领域:
催化化学
·
理论计算化学
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产品关联
DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2023
·
IF 10.4
Ruizhe Chen,Leilei Cheng,Jing Gu,Haoran Yuan,Yong Chen
Hydroconversion has been demonstrated as a viable method to efficiently deconstruct polyolefins under relatively mild conditions. The hydrogenolysis of C–C bonds over Ru-based catalysts can convert polyolefins into liquid alkanes and methane. To suppress methane generation and obtain high-value isomer, further exploration of the mechanism for the cooperative deconstruction of polyolefins by bifunctional catalysts with metal–acid sites is necessary. In this study, we utilized ball milling to enhance the accessibility of acid sites within MOR zeolite, while the fragmented pore structure ensured that the loaded Ru metal was sufficiently accessible for long-chain alkanes. The sequential accessibility of metal–acid sites boosted the hydroconversion efficiency of low-density polyethylene (LDPE). Through systematic investigations involving catalysts with various Ru loadings and Si/Al ratio of zeolites, it is discovered that the smaller-sized Ru particles not only facilitate the generation and desorption of olefinic intermediates in hydrocracking but also promote the hydrogenation and desorption of alkyls and suppress the cascade of terminal C–C bond cleavage in hydrogenolysis. Liquid fuel (C 5 -C 21 ) yield was increased by 27% for the catalyst loaded with 0.7 wt% Ru on mMOR20 compared to 1.7 wt% loadings, while methane yield was only one-third of the latter. Concurrently, the distribution of acid sites on the zeolite surface affected the aggregation process of Ru atoms. This study deeply unveils the synergistic interaction of metal–acid sites, facilitating internal C–C bond cleavage to obtain liquid fuel and sheds light on catalyst design for waste polyolefins upcycling.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）