ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Feng Long,Xincheng Cao,Xia Jiang,Peng Liu,JianChun Jiang,Xiaolei Zhang,Junming Xu
Catalyst design is critical for renewable selective hydrogenation of fatty acids into alkanes or alcohols, especially for active metals and supports. We demonstrate that NiCu anchored on a TiO2 (P25) surface, prepared by the impregnation method, performed superior temperature-sensitive catalytic activities with a higher fatty alcohol yield of 78.2% (205 °C, 4 MPa H2, and 12 h) and alkane yield of 85.0% (245 °C, 3 MPa H2, and 6 h). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) suggest that Ni or NiCu anchored on rutile with oxygen vacancies can achieve reversal of charge transfer between the metal and TiO2 support. Especially, the normal NiCu cluster loading on the rutile surface can improve the dispersion of the NiCu cluster and oxygen vacancy concentration. Thus, more NiCu clusters anchored on oxygen defects can obtain negative charges in favor of alcohol production. In contrast, the other active NiCu clusters will preferentially cleave the C–C bond to produce alkanes at a higher reaction temperature. Our work provides a new strategy for designing highly effective hydrogenation catalysts.
研究领域:
催化化学
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材料科学
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可再生能源
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2025
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IF 6.5
Chengliang Wang,Xia Guo,Jinbian Lv,Yin Zhang,Haitao Li,Jie Gao,Wei Wei,Di Zhang,Yongxiang Zhao
The primary products of the direct hydrogenation of Maleic Anhydride (MA) are Succinic Anhydride (SAH) and γ-butyrolactone (GBL). Achieving selective synthesis of these products by regulating the composition, structure, and textural properties remains a focal point in the research field of maleic anhydride hydrogenation. Based on the characteristic of atomic level uniform distribution of cations of layered double hydroxides (LDHs), a highly loaded, highly dispersed and homogenized NiCu alloy bimetallic catalyst was synthesized using NiCuAl-LDHs as precursor. Compared with Ni/Al 2 O 3 catalyst derived from NiAl-LDHs, the introduction of Cu can effectively improve the hydrogenation activity of C=C bonds while inhibiting the hydrogenolysis of C=O bonds. Under identical reaction conditions, the primary product of the Ni/Al 2 O 3 catalyst was γ-butyrolactone (GBL) with a yield of 94.2 %, whereas the primary product of the NiCu 0.4 /Al 2 O 3 catalyst was Succinic Anhydride (SAH) with a yield of 90.5 %. The introduction of Cu resulted in the formation of a homogeneous NiCu alloy phase in the catalyst, which significantly influenced the adsorption configurations and adsorption energies of the reactants and intermediates. This effect can be attributed to the electronic interactions between Ni and Cu, which shift the d-band center of Ni away from the Fermi energy level, thereby facilitating the directed synthesis of Succinic Anhydride (SAH) and γ-butyrolactone (GBL). These findings were confirmed by various characterization techniques and DFT theoretical calculations. Future catalyst development in maleic anhydride hydrogenation will significantly benefit from the design approach and research ideas presented in this study.
研究领域:
催化化学
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材料科学
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理论计算化学
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2025
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IF 5.3
Dekang Li,Zhixian Bao,Lijun Jin,Haoquan Hu
Dry reforming of methane (DRM) can spontaneously use CO2 and CH4 to produce syngas, but minimal sulfur impurities in the feed gas can poison and deactivate the catalyst. Although the Ni/Al2O3 catalyst has excellent DRM activity, it is challenging to regenerate due to sulfation of the support. Besides that, the loading of sacrificial promoters used to improve sulfur resistance, such as Cu, may impact the DRM performance of active sites. Here, a spatial separation strategy was proposed to precisely design a sulfur-resistant catalyst, dividing the catalyst into a DRM zone and a H2S adsorption zone. The Ni@SiO2@NiCu catalyst prepared by this strategy shows stable DRM performance and significantly improved sulfur resistance and can be regenerated repeatedly. The Ni@SiO2@NiCu catalyst has the best sulfur resistance, 6.8 times that of the spatially adjacent NiCu@SiO2 catalyst and 1.4 times that of the Ni@SiO2@Cu catalyst. This spatial separation strategy introduces a novel concept for the controllable synthesis of sulfur-resistant catalysts and may inspire further applications in the design and development of such catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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环境科学
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能源技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2023
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IF 4.7
Riyang Shu,Yuankai Lin,Linxuan Zhou,Bowen Luo,Sheng Yang,Zhipeng Tian,Chao Wang,Zhengjun Shi,Ripsa Rani Nayak,Navneet Kumar Gupta
Bimetallic catalysts are widely favored for catalytic reactions due to their superior performance and cost-effectiveness. This study delves into the utilization of a non-noble bimetallic catalyst, NiCu/C, in the hydrogenolysis of lignin to yield valuable aromatic monomers. Under optimized temperature, this catalyst achieves an impressive 92.4% conversion of lignin into liquid products, yielding 17.7 wt% of monomers. These results outperform the performance of the monometallic catalysts (Ni/C and Cu/C). To gain insight into the detailed catalytic reaction mechanism, the catalysts underwent advanced characterization techniques such as N 2 physisorption, XRD, XPS, H 2 -TPR, and TEM, which provided information on their textural properties, structure, oxidation states, and more. The findings clearly highlight the significant role played by the synergistic interaction between Ni and Cu metallic species in bolstering the H 2 adsorption capacity, thereby resulting in elevated catalytic hydrogenolysis activity. Characterization of the lignin hydrogenolysis products was also conducted to understand the effects of bimetallic and monometallic catalysts. These findings align with the catalyst characterizations and lend further support to the significant enhancement in catalytic hydrogenolysis attributed to the synergistic impact of the NiCu/C catalyst.
研究领域:
化学工程
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催化
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子