Journal of Energy Chemistry
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2022
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IF 13.599
Weizhen Xie,Binglin Chen,Wenlong Jia,Huai Liu,Zheng Li,Shuliang Yang,Xing Tang,Xianhai Zeng,Yong Sun,Xixian Ke,Tianyuan Li,Huayu Fang,Lu Lin
Developing an efficient and easily available catalyst for the selective conversion of biomass-derived 5-hydroxymethylfurfural (HMF) into furan-2,5-dimethylcarboxylate (FDMC), a valuable biomass-based monomer, remains a high demand but formidable challenge. Herein, a facile strategy for the synthesis of N-doped carbon-supported Co/Fe bimetallic catalyst (CoFe-NC) was developed, which provided an outstanding FDMC yield of 93% in a batch reactor (base-free, 80 °C, 2 bar O 2 , 4 h). Interestingly, CoFe-NC also gave a high FDMC yield of 91% under continuous-flow conditions for 80 h (5 bar O 2 , 80 °C, GHSV 1320 h −1 , LHSV 0.6 h −1 , base-free). Notably, it is the first time that a non-noble catalyst gave such a high FDMC yield under continuous-flow conditions. The introduction of Fe could greatly improve both the electron intensity of Co-N x species and basicity of the catalyst, which endowed CoFe-NC with improved O 2 activation capacity and enhanced dehydrogenation activity for the oxidation-esterification of HMF. This work delineates the efficient strategy on the construction of N-doped carbon-supported non-noble catalyst, which might open a new avenue for developing highly efficient catalyst for FDMC production.
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ACS Applied Materials & Interfaces
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2021
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IF 9.229
Xing Yuan,Lingquan Meng,Chaohe Zheng,Haibo Zhao
Perovskites have been recognized as affordable substitutes for noble-metal catalysts for their tunable catalytic activity and thermal stability. Nevertheless, the highly demanding synthesis procedure still hinders the application of perovskites in catalytic combustion. In this work, a series of nanostructured SiTiO3 perovskites with B-site partial substitution by Co, Fe, Mn, Ni, and Cu are synthesized via flame spray pyrolysis in one step. The comprehensive characterizations on textural properties of nanostructured perovskites reveal that the flame-made perovskite nanoparticles all exhibit high crystal purity and large specific surface area (∼40 m2/g). Furthermore, the highest catalytic activity is achieved by SrTi0.5Co0.5O3 due to the formation of favorable oxygen vacancies, outstanding reducibility, and oxygen desorption capability. Additionally, the presence of 10 vol % water vapor during long-term testing indicates remarkable durability and water resistance. Finally, the CO oxidation and CH4 dehydrogenation on SrTiO3 incorporating Co atoms are more thermodynamically and kinetically favorable than those on other doped surfaces.
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PubMed
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Catalysis Science & Technology
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2024
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IF 4.4
Zhicheng Xu,Jin Xiong,Yuran Li,Junxiang Guo,Bin Wang,Tingyu Zhu
For industrial flue gas purification at medium and low temperatures, it is highly necessary to promote the denitrification activity of V-based catalysts in a SO2 atmosphere. Transition metals (Ce, Co, Fe, and Mn) are used to modify V/Ti catalysts to improve SO2 resistance with ammonium bisulfate deposition on the catalysts. Sulfation on Ce with less ammonium bisulfate deposition considerably improves the SO2 resistance of V1Ce5/Ti, and stable sulfation on TiO2 promoted by Co provides additional Brønsted acid sites for V1Co5/Ti to reduce the deactivation. Serious sulfation on V1Mn5/Ti with large ammonium bisulfate deposition on V1Fe5/Ti causes deeper deactivation. The formation mechanism of ammonium bisulfate on active metal sites and TiO2 carriers has been clarified. SO2 is adsorbed on V sites and transition metal sites followed by oxidation and ammoniation or adsorbed on TiO2 carriers followed by ammoniation and oxidation. The first pathway is more dominant than the second pathway in the presence of O2 with the co-oxidation of SO2 by O2 and lattice oxygen. The initial formation temperature and stable temperature of dominant intermediates were determined by in situ DRIFTS. SO2 adsorbed on TiO2 carriers is oxidized by V sites above 170 °C to form a tridentate sulfate, while SO2 adsorbed on transition metal sites is initially oxidized by transition metal sites above 50 °C to form monodentate and bidentate sulfates, as well as competitively oxidized by V sites above 170 °C to form tridentate sulfates. The selective adsorption of SO2 on transition metal sites or TiO2 carriers and the competitive oxidation of SO2 by transition metal sites and V sites provide a synergistic effect between V sites and transition metal sites to reduce ammonium sulfate deposition and release more active sites. These findings provide theoretical guidance to design and prepare V-based catalysts with high denitrification activity in the presence of SO2.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 47
·期 3
·1156-1164
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IF 3.925
Li-Jing Peng,Shi-Jun Yin,Li Chen,Tao Tian,Wei-Yi Zhang,Hang-Yu Zhou,Feng-Qing Yang
Herein, a Co–Fe Prussian blue analogue nanocube (Co–Fe PBA NC) was prepared in situ via a simple and rapid coprecipitation method at room temperature, and the synthesized nanocube was systematically characterized. The Co–Fe PBA NC was proven to have intrinsic oxidase-like activity, which can catalyze the production of reactive oxygen species, such as superoxide anions (O2˙−), hydroxyl radicals (˙OH), and singlet oxygen (1O2), in a dissolved oxygen system without the presence of hydrogen peroxide (H2O2). By making full use of the oxidase-like activity of the Co–Fe PBA NC and using the chromogenic substrate 3,3′,5,5′-tetramethylbenzidine (TMB), a colorimetric sensor was fabricated for the detection of ascorbic acid (AA) and its related biological enzymes’ activities, including alkaline phosphatase (ALP), α-glucosidase (α-Glu), and ascorbic acid oxidase (AAO), in human serum. This study presents an oxidase mimic that can be synthesized via a simple, rapid, and low-cost method, which overcomes the defects of cumbersome and time-consuming synthetic process, dependence on professional instruments and high cost of some previously reported nanozymes. In addition, this study provides a new multifunctional colorimetric sensing platform for AA and its related biological enzymes, showing great potential in biological assays.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Sundaram Chandrasekaran,Na Li,Yang Zhuang,Lijun Sui,Zhizhong Xiao,Dayong Fan,Vanchiappan Aravindan,Chris Bowen,Huidan Lu,Yongping Liu
The creation of heterostructures based on non-precious metals with platinum-like hydrogen evolution reaction (HER) performance remains a challenge for hydrogen fuel technologies. Motivated by the fascinating properties of heterostructures, we establish here an effective approach to fabricate the heterostructured M−N−Ni 9 S 8 /Nb 2 O 5 ( M = Co, Fe, or Cu) catalysts using spatially separated Ni 9 S 8 nanosheet/Nb 2 O 5 nanobelts that are coupled with nitrogen (N) and metal atoms. Due to its improved intrinsic activity, interface-rich structure, abundant active sites, and large surface area the Co−N−Ni 9 S 8 /Nb 2 O 5 heterostructure achieved a low acidic HER overpotential of −171 mV at −10 mA cm −2 , thereby performing better than existing heterostructures. Moreover, for the alkaline HER, the Cu−N−Ni 9 S 8 /Nb 2 O 5 heterostructure required a low overpotential of −109 mV at −10 mA cm −2 , which is close to the performance of Pt/C catalyst. Density functional theory (DFT) predictions indicate that the local charge distribution and electronic properties at the heterointerface of Ni 9 S 8 /Nb 2 O 5 can be significantly modulated by co-doping of metals with N atoms, resulting in optimal adsorption energy and reduced water dissociation barrier; thereby accelerating the acidic and alkaline HER activity. This work, therefore, provides a new design principle to create advanced heterostructured catalysts.
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