DALTON TRANSACTIONS
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2025
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IF 3.3
Xue-Qing Xu,Shen Yu,Xing-Yu Yue,Zhan Liu,Jia-Min Lyu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
Phenol is an important intermediate for high value chemicals. Current phenol production via a three-step cumene process causes severe energy-waste and environmental problems. The conversion of benzene to phenol under mild condition can be achieved by oxidation with Cu-based zeolites. However, conventional microporous zeolite suffers from severe diffusion limitation, especially when bulky molecules are involved, such as benzene. In this work, we used a hierarchically macro-meso-microporous ZSM-5 single crystal (Hier-ZSM-5) as substrate for Cu species (Cu@Hier-ZSM-5). Irregular morphology of opal-like Hier-ZSM-5 exhibits abundant surface Si-OH groups and provides a platform for stabilizing Cu2+ sites. Meanwhile, hierarchical porosity provides significantly improved diffusion ability of bulky molecules. As a result, excellent selective oxidation performance of benzene was obtained with the Cu@Hier-ZSM-5, achieving a conversion of 77% and a phenol selectivity of 73%, which is 1.5 times and 2 times of these obtained with a catalyst based on a microporous ZSM-5, respectively. Species of CuOOH were identified as an important intermediate for benzene oxidation. This hierarchical zeolite system with a synergistic effect of site anchoring and molecular diffusion presents an excellent platform for catalyst design.
研究领域:
催化化学
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材料科学
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环境化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Zhen Zhang,Jiang Wu,Bin Li,Huibin Xu,Dongjing Liu
Zeolite (ZSM-5), as a kind of carbon-free sorbent or catalyst, has been widely applied in many fields due to its big surface area, good chemical and thermal stability, and excellent adsorption performance. In this study, Mn-Fe modified ZSM-5 are synthesized via sol-gel approach and employed for elemental mercury (Hg 0 ) removal from simulated flue gas at low temperature. The results show that pure ZSM-5 shows poor mercury capture ability with Hg 0 removal efficiency of ~8.5–18.8% at 100–300 °C. Mn or Fe modification can both efficiently enhance the Hg 0 removal efficiency of the ZSM-5. The sorbent with Mn/Fe molar ratio of 1:2 exhibits the optimal mercury capture ability with the highest Hg 0 removal efficiency near 100% at temperatures of 200 and 250 °C due to the significant synergy effect between Mn 2 O 3 and Fe 2 O 3 . The presence of NO has a negligible effect on the Hg 0 removal performance of Mn/ZSM-5 and Mn1Fe2/ZSM-5, while the existence of SO 2 considerably degrades the Hg 0 capture performance of Mn/ZSM-5 owing to competing adsorption and side reactions. Fe addition can protect Mn active sites from SO 2 poisoning and thereby enhancing the SO 2 resistance of Mn/ZSM-5 to some extent.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
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2021
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IF 7.086
Jinyu Hou,Daoxu Zhong,Wuxing Liu
Hazardous oil sludge (OS) poses a great challenge to the environment, whereas conventional treatment methods (i.e., incineration or pyrolysis-incineration) are relatively less value-added and will bring about air pollution problems. To realize the high-value utilization of OS, catalytic co-pyrolysis with waste biomass to produce platform chemicals was studied using TG-FTIR and Py (pyrolyzer)-GC/MS methods. Results showed that for the non-catalytic co-pyrolysis of RH (rice husk) and OS, the main synergy on weight loss was the greatly lowered initial pyrolysis temperature of RH (for ∼55 °C) at the lower temperatures and the reduced weight loss ratio of OS (∼10–18 wt%) within the higher temperature range. ZSM-5 catalyst promoted the degradation of OS and RH mixtures at < 150 °C, yet showed minor effects on their weight loss at higher temperatures. The oxygenated and aliphatic compounds from non-catalytic co-pyrolysis were efficiently converted, resulting in an increased relative yield of aromatics to the highest of 46% and an elevated selectivity to BTX (as high as 60%). Despite the relatively short carbon chain length of OS components, ZSM-5 was proved effective to activate the OS pyrolysis products, thus enhancing the further aromatization reactions with biomass pyrolysis intermediates. This study provides a novel method for value-added co-utilization of hazardous OS waste and abundant biomass waste, and thus is beneficial to producing renewable chemicals while reducing the environment pollutant.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Haotian Guo,Xinhuan Lu,Jie He,Huaxin Zhang,Haifu Zhang,Yanhong Dong,Dan Zhou,Qinghua Xia
A composite material ZSM-5@Co-MOF containing Co-MOF and ZSM-5 was successfully prepared by steam-assisted crystallization of Co-MOF on the zeolite surface. Compared to physically mixing Co-MOF on the zeolite surfaces, Co-MOF nanosheets were uniformly attached to external surfaces of the ZSM-5 crystals because of the enhanced interaction between zeolite and Co-MOF in the composite. In addition, the Co-MOF was distributed as a nanosheet structure, and its dispersibility was greatly enhanced, in which this behavior led to more uniform distribution of the deposited active sites. Interestingly, the designed composite exhibited an excellent catalytic performance for the epoxidation of α-pinene with air. Compared to isolated Co-MOF and ZSM-5, high yield of the product (94.4%) was obtained over the 0.5ZSM-5@Co-MOF-150 composite due to the highly dispersed Co-MOF nanosheet. This opens up interesting prospects for developing new zeolite@MOF composite catalysts as efficient heterogeneous catalysts.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Feng Ye,Shuanshi Fan,Xuemei Lang,Yanhong Wang,Yihui Lv,Gang Li
Developing hierarchical zeolites is highly important for catalytic applications. In this study, micro- and submicron-sized hierarchical ZSM-5 zeolites, composed of aggregated nanosized ZSM-5 crystals, were facilely synthesized without any mesoporogen. The effects of the gel composition in a mesoporogen-free system on the formation of ZSM-5 aggregates were studied. The results revealed that the Na 2 O/SiO 2 molar ratio and the aluminum source exerted significant impacts. Furthermore, we demonstrated that the morphology and size of the ZSM-5 aggregate could be easily adjusted by varying the gel composition. Mechanistic insights indicated that the formation of hierarchical ZSM-5 aggregates in the mesoporogen-free system likely followed a space-confined growth mechanism.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
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2021
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IF 8.001
Feng Lin,Yulong Ma,Yonggang Sun,Kanghe Zhao,Tingting Gao,Yingbo Zhu
Due to the inertness and structural complexity of lignin, upgrading lignin to biofuels and fine chemicals still faces great challenges. In this paper, a one-pot method was used to catalyze straw lignin with H-ZSM-5 supported by Ni and Ru bimetals, and the lignin conversion rate reached 88.1%. The yield of monophenol was 19.5%, of which the yield of 4-ethylphenol and 4-ethylguaiacol was 4.9% and 3.8%, respectively. The 2D HSQC NMR analysis confirmed that the Ni–Ru/H-ZSM-5 catalyst had an obvious activity of breaking C β -O bonds before and after the reaction. The result showed that after loading metal Ni and Ru, the Lewis acid of the catalytic system was greatly increased, which caused electron transfer between Ni and Ru. 3Ni-1.5Ru/H-ZSM-5 had the strongest activity due to the largest synergy among Ni, Ru and H-ZSM-5. The synergy was the key factor leading to the cleavage of C–C and C–O bonds in straw lignin and the high-performance catalytic degradation of lignin. Besides, the effect of reaction solvent and hydrogen resource on upgrading lignin to fine chemicals over 3Ni-1.5Ru/HZSM-5 catalyst was also intensively investigated. This research developed a method for the direct conversion of lignin into valuable monophenols.
研究领域:
催化化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2019
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IF 3.372
Piao Liu,Jianxin Cao,Zheng Xu,Chunliang Yang,Xiaodan Wang,Fei Liu
Core-shell structured ZSM-5@t-ZrO 2 catalysts were prepared by a hydrothermal coating method, and their physicochemical properties, catalytic performance, and deactivation behavior in thiolation reactions were studied using a ZSM-5/t-ZrO 2 physically-blended catalyst as a comparison. Reactions using the core-shell ZSM-5@t-ZrO 2 catalyst were carried out at a pressure of 0.7 MPa, 370 °C, a H 2 S:CH 3 OH molar ratio of 2:1, and a N 2 flow rate of 90 ml·min −1 . The conversion of CH 3 OH, and the selectivity and yield of CH 3 SH under these conditions were 92.07%, 90.89%, and 83.68%, respectively, and the catalytic lifetime was longer than 30 h. Compared with the ZSM-5/t-ZrO 2 physically-blended catalyst, the CH 3 SH yield and the catalytic lifetime of the core-shell structured ZSM-5@t-ZrO 2 catalyst were higher by 5.37% and 150%, respectively. The unique reaction pathway of the shell (t-ZrO 2 , Lewis (L) base active site)-core (ZSM-5, Brǿnsted (B) acid active site) and the Lewis-Brønsted acid active center based on a composite solid-solution interface were mainly responsible for the high activity of the thiolation reaction. Meanwhile, the formation of a micro-mesoporous system increased the diffusion of molecules and reduced the deactivation rate of carbon- and sulfur-containing deposits. Generally, carbon- and sulfur-containing substances deposited on catalysts were mainly composed of polymethylbenzene, polymethyl naphthalene, cyclic elemental sulfur, and other compounds containing C S and S S bonds. Finally, the core-shell structured catalysts showed excellent resistance to deactivation by carbon- and sulfur-containing deposits.
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
CATALYSIS TODAY
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2020
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IF 5.825
Hong Du,Miao Jiang,Xiuyun Ma,Peifang Yan,Z. Conrad Zhang
The rapid consumption of fossil resources and the grim environmental situation encourage the application of renewable and clean energy resources. Conversion of biomass, which is a kind of renewable, CO 2 neutral as well as abundant reserves carbon containing resource, is significantly important. The production of fuels from biomass by means of gasification and Fischer-Tropsch synthesis is one of the most promising routes for industrial applications. The wax-free liquid fuels synthesis directly from H 2 -deficient syngas similar to bio-gas is highly advantageous for reducing investment and operating cost. Thus, the Mn-promoted meso-ZSM-5 supported cobalt catalyst was applied for the production of wax-free liquid fuels by catalytic H 2 -deficient syngas conversion in this study. The performance of the reaction was influenced obviously by Mn content. The cobalt dispersion increased with the addition of Mn, whereas the reduction degree decreased after Mn doping. Then, the balance between the dispersion and reduction degree led to the change in CO uptake followed a volcanic curve. The catalyst with moderate amount of Mn (1 wt%) had the suitable cobalt particle size and the maximum CO uptake. Thus, the highest CO conversion was obtained over Co-1Mn/meso-ZSM-5 catalyst thanks to its maximum exposed active sites. The appropriate amount of Mn addition also resulted in the decreasing of CH 4 selectivity. The highest space time yield of liquid fuels was acquired over the Co-1Mn/meso-ZSM-5 catalyst from H 2 -deficient syngas conversion under the moderate conditions.
研究领域:
能源化学
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催化反应工程
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2019
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IF 6.669
Lin Jiang,Yunpu Wang,Leilei Dai,Zhenting Yu,Qi Yang,Sha Yang,Deyu Jiang,Zhiyun Ma,Qiuhao Wu,Bo Zhang,Yuhuan Liu,Roger Ruan
A ZSM-5/SiC composite catalyst was synthesized and characterized by Brunauer–Emmett–Teller analysis, X-ray diffraction, and scanning electron microscopy in this study. The composite catalyst had the characteristics of ZSM-5 and SiC, and the surface of SiC grew evenly with a layer of ZSM-5. The effect of the composite catalyst on the product distribution and chemical composition in a co-pyrolysis downdraft system was investigated. In a down system with a catalytic temperature of 450 °C, a feed-to-catalyst ratio of 2:1, and a soybean-soapstock-to-straw ratio of 1:1, the proportions of alkanes, olefins, aromatics, and phenoxy compounds were 6.82%, 4.5%, 73.56% and 11.11%, respectively. The composite catalyst combined the catalytic performance of ZSM-5 and SiC, increasing the proportion of aromatics and decreasing the proportion of oxygen-containing compound in the bio-oil. Moreover, the composite catalyst maintained its activity after reusing several times.
研究领域:
能源与环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2019
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IF 7.723
Xiaoyue Wan,Qi Zhang,Mingming Zhu,Yi Zhao,Yongmei Liu,Chunmei Zhou,Yanhui Yang,Yong Cao
Site-selective deoxygenation of hydroxyl groups represents essential processes to access valuable functionalized bio-based compounds with industrial potential. One of the challenging tasks in this context is to convert biodiesel-derived glycerol in the presence of abundant water directly to 1,3-propanediol (1,3-PDO), a key component of the emerging polymer industry. Herein, a monometallic iridium supported on H-ZSM-5 in the absence of Re oxophilic metal oxides was prepared via grinding-assisted impregnation procedures and attempted as an effective and recyclable catalyst for the aqueous-phase selective hydrogenolysis of glycerol toward 1,3-PDO in the absence of acid additives. The results revealed the necessity to control the Ir domain dispersions, Ir 0 /Ir 3+ ratio and the amounts of overall acid/Brönsted acid sites. Activity depended linearly on the amount of overall and Brönsted acid sites, and 1,3-PDO selectivity increased in the presence of Ir-induced Brönsted acid sites, denoted as Ir-O(H)-H-ZSM-5. We speculate that Ir-O(H)-H-ZSM-5 are generated by the interfacial synergistic interaction between IrO x and H-ZSM-5 through hydrogen spillover and reverse hydrogen spillover according to the reported literatures. The reaction mechanism to elucidate the role of Ir-O(H)-H-ZSM-5 sites in glycerol hydrogenolysis was also postulated based on extensive characterization and catalytic reaction results.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Qin Zhu,Jiaorong Yan,Qiguang Dai,Qingqing Wu,Yuanpu Cai,Jinyan Wu,Xingyi Wang,Wangcheng Zhan
A unique zeolite catalyst, Fe doped ZSM-5 microsphere assembled by uniform nanorod-like crystals with hierarchical pore structure, was successfully synthesized and applied for the adsorption and degradation of trace chlorobenzene (CB) in the presence of H 2 O 2 . The organic ferric salts as the precursors, ethylene glycol as a chelating/reducing agent and the dynamic two-stage temperature-varied hydrothermal technique, together made the synthesized hierarchical Fe-ZSM-5 nanorods assembled microspheres (FZ-CA-5EG) to be characterized by abundant highly dispersed and valency-controlled framework Fe 3+/2+ species. As a result of these features, the FZ-CA-5EG showed excellent ability of adsorption and degradation efficiency of CB, and enhanced durability due to negligible leaching of framework Fe species. Moreover, the hydroxyl radicals were determined as the main the reactive oxygen species of CB oxidation degradation, and a possible adsorption-oxidation degradation pathway was proposed.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RENEWABLE ENERGY
·
2023
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IF 8.7
Mengxue Song,Chonghao Qiu,Pengfei Ma,Jiawei Zhong,Zhuohan Zhang,Weiping Fang,Wenjing Song,Jianqiang Fan,Weikun Lai
Reductive etherification is an attractive and practical strategy to convert bio-platform compounds into valuable chemicals. In directed synthesis of furfuryl ethers, reductive etherification of bioderived furfurals is still challenging due to the complexity of catalytic reaction . Herein, reductive etherification of furfural with alcohol was investigated over Ni/ZSM-5 catalyst, which found that Si/Al ratios in ZSM-5 played an important role on the catalytic performance. For Ni/ZSM-5 with Si/Al ratio of 50, 80.9% yield of furfuryl ether at 90.8% conversion of furfural was achieved under the condition of 2 MPa H 2 and 180 °C for 3 h in isopropanol. The catalyst exhibited superior stability and recyclability during the consecutive cycle run. Catalysts characterization demonstrated that both acidic properties and furfural adsorption were influenced by the Si/Al ratios in Ni/ZSM-5, which correlated to the reaction route and catalytic performance. Lewis acid sites enhanced furfural hydrogenation into furfuryl alcohol, while Brønsted acid sites on ZSM-5 effectively catalyzed sequential etherification of furfuryl alcohol to furfuryl ether. Under optimization conditions, various furfuryl ethers could be obtained with yields above 80% over Ni/ZSM-5 catalyst in different primary alcohols, demonstrating the general versatility of the approach. Our findings offered opportunities to develop an efficient furfuryl ethers synthesis method .
研究领域:
催化化学
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能源化学
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绿色化学
✓ 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）