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学者姓名:员汝胜
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MXene species have emerged as a class of compelling electrode materials in the field of capacitive deionization (CDI). However, as an excellent member of the MXene family, the Nb4C3Tx has not received much attention in terms of CDI. Herein, we have not only established the feasibility of Nb4C3Tx as a potential desalination electrode materiel but also proposed a wrinkle-engineering strategy that can effectively improve the CDI performance of Nb4C3Tx freestanding membranes. Specifically, the introduction of wrinkles on Nb4C3Tx nanosheets contributes to optimizing the interlayer space, accessibility, conductivity, stability, and CDI performance of the assembled membranes. In particular, the optimized wrinkled Nb4C3Tx membranes can achieve an ultrahigh desalination capacity of similar to 188.2 mg g(-1) at 1.6 V accompanied by a fast adsorption rate of similar to 12.6mg g(-1) min(-1), showing great competitiveness with other MXene individual electrodes. In addition, the as-designed electrodes also exhibit superior cycle desalination stability as well as good applicability to different salts (such as LiCl, KCl, CaCl2, and MgCl2). This work both extends the MXene material applicable to CDI and offers an effective solution for improving the properties of Nb4C3Tx-MXene lamellar membrane electrodes, opening up enormous opportunities for the use of such MXene species in the field of electrochemical desalination.
Keyword :
Capacitive deionization Capacitive deionization Faradaic electrodes Faradaic electrodes Freestanding membranes Freestanding membranes Nb4C3Tx Nb4C3Tx Wrinkle-engineering Wrinkle-engineering
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GB/T 7714 | Liu, Haoyang , Shang, Jing , Liu, Liyan et al. Capacitive deionization using wrinkle-engineered Nb4C3Tx-MXene freestanding membranes [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 507 . |
MLA | Liu, Haoyang et al. "Capacitive deionization using wrinkle-engineered Nb4C3Tx-MXene freestanding membranes" . | CHEMICAL ENGINEERING JOURNAL 507 (2025) . |
APA | Liu, Haoyang , Shang, Jing , Liu, Liyan , Yuan, Rusheng , Long, Jinlin , Xu, Chao . Capacitive deionization using wrinkle-engineered Nb4C3Tx-MXene freestanding membranes . | CHEMICAL ENGINEERING JOURNAL , 2025 , 507 . |
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The doping of metals onto the inorganic non-metallic catalyst g-C3N4 facilitates the reduction of CO2 to C1 and C2 products, representing an effective method for reducing atmospheric carbon dioxide and mitigating global warming. This paper investigates the stability and catalytic activity of g-C3N4 doped with Fe, Co, Ni, and Cu using density functional theory (DFT). The optimal reduction pathways of CO2 at different metal sites are analyzed. The results show that bimetallic doping exhibits a synergistic effect compared to traditional metal doping, significantly enhancing the visible light response range of g-C3N4, promoting the adsorption and activation of CO2, and lowering the Gibbs free energy barrier of the reduction intermediates. Of the materials studied, Co2@g- C3N4 and Ni2@g-C3N4 require higher energy and show poor CO2 activation performance. In contrast, Fe2@g- C3N4's site1 and site2 display superior catalytic performance with activation energy barriers of 0.74 eV and 0.78 eV, respectively. Cu2@g-C3N4, on the other hand, shows favorable performance only at site1, with an activation energy barrier of 0.63 eV. This catalyst is expected to serve as an effective tool for CO2 reduction, providing a new strategy for the design and development of more efficient and selective CO2 reduction catalysts.
Keyword :
C 2 products C 2 products CO 2 reduction CO 2 reduction Dual-atom catalysts Dual-atom catalysts First-principles calculation First-principles calculation Graphite carbon nitride Graphite carbon nitride
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GB/T 7714 | Hu, Xiaoyi , Li, Qingyu , Li, Weiguo et al. Spin-polarized binuclear transition metal doping on g-C3N4 for photocatalytic CO2 reduction to C2 products: A DFT study [J]. | MOLECULAR CATALYSIS , 2025 , 572 . |
MLA | Hu, Xiaoyi et al. "Spin-polarized binuclear transition metal doping on g-C3N4 for photocatalytic CO2 reduction to C2 products: A DFT study" . | MOLECULAR CATALYSIS 572 (2025) . |
APA | Hu, Xiaoyi , Li, Qingyu , Li, Weiguo , Deng, Yixin , Liu, Diwen , Zhang, Yanjie et al. Spin-polarized binuclear transition metal doping on g-C3N4 for photocatalytic CO2 reduction to C2 products: A DFT study . | MOLECULAR CATALYSIS , 2025 , 572 . |
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The valorization of native lignin to functionalized aromatic compounds under visible light is appealing yet challenging. In this communication, colloidal mercaptoalkanoic acid capped ultrathin ZnIn2S4 (ZIS) microbelts was successfully fabricated, which was used as a superior catalyst for depolymerization of native lignin in birch woodmeal under visible light, with an optimum yield of 28.8 wt % to functionalized aromatic monomers achieved in 8 h. The capped mercaptoalkanoic acid not only enables a solvent modulated reversible interchange of ZIS between the colloidal state for efficient reaction and the aggregated state for facile separation, but also serves as a precursor for light initiated generation of reactive thiyl radical for highly selective cleavage of β-O-4 bond in native lignin. This work provides a green and efficient strategy for the depolymerization of native lignin to functionalized aromatic monomers under mild conditions, which involves a new mechanism for the cleavage of β-O-4 bonds in native lignin. The capability of cleavage of β-O-4 bonds in native lignin by photogenerated thiyl radicals also demonstrates the great potential of using photogenerated thiyl radicals in organics transformations. © 2024 Wiley-VCH GmbH.
Keyword :
Depolymerization Depolymerization Heterogeneous Catalysis Heterogeneous Catalysis Lignin Lignin Photochemistry Photochemistry Radicals Radicals
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GB/T 7714 | Wang, J. , Li, Y. , Liu, H. et al. Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical [J]. | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
MLA | Wang, J. et al. "Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical" . | Angewandte Chemie - International Edition 63 . 37 (2024) . |
APA | Wang, J. , Li, Y. , Liu, H. , Ding, Z. , Yuan, R. , Li, Z. . Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical . | Angewandte Chemie - International Edition , 2024 , 63 (37) . |
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A 2D Mn-based MOF ([Mn4(PDI)2(DMF)7(H2O)]n (MOF 1)) (H4PDI = 5,5 '-(1,3,6,8-tetraoxo-1,3,6,8-tetrahydrobenzo[lmn][3,8]phenanthroline-2,7-diyl)diisophthalic acid) was synthesized. Visible light excited Mn-PDI unit in MOF 1 oxidizes NaSO2CF3 to generate center dot CF3 radical and enables MOF 1 to exhibit activity for trifluoromethylation of (hetero)arenes under visible light. The unusual stability of MOF 1 in the trifluoromethylation reactions can be attributed to its unique structure, which prevents it from corrosion by acid byproduct. The peeling of MOF 1 to ultrathin nanosheets or partial oxidation of Mn(II) to Mn(III) in MOF 1 led to MOL 1 and NB 1 with significant improved activity for trifluoromethylation reactions, demonstrating the important role of composition and morphology of a catalyst on its performance. The light initiated trifluoromethylation reactions over these Mn-based MOFs was applied to a variety of substrates. This study provides an efficient strategy for synthesis of trifluoromethylated compounds and highlights the potential of MOFs in light initiated organic syntheses.
Keyword :
Acid tolerance Acid tolerance CF 3 radicals CF 3 radicals Mn-based MOF Mn-based MOF Photocatalysis Photocatalysis Trifluoromethylation Trifluoromethylation
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GB/T 7714 | Ma, Xiong-Feng , Wen, Bo , Zhang, Shaohui et al. Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction [J]. | JOURNAL OF CATALYSIS , 2024 , 436 . |
MLA | Ma, Xiong-Feng et al. "Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction" . | JOURNAL OF CATALYSIS 436 (2024) . |
APA | Ma, Xiong-Feng , Wen, Bo , Zhang, Shaohui , Wang, Deshun , Wang, Lele , Lin, Huaxiang et al. Stable Mn(II) metal-organic framework for efficient visible light initiated trifluoromethylation reaction . | JOURNAL OF CATALYSIS , 2024 , 436 . |
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Converting clean solar energy into chemical energy through artificial photosynthesis is an effective solution to solve the energy and environmental issues. Here, we report a Cs3Bi2Br9/Bi2WO6 (CBB/BWO) Z-scheme heterojunction constructed via electrostatic self-assembly, which facilitates efficient separation of photogenerated carriers and ensures the corresponding redox capacity of both components. By sharing Bi atoms, a Br-Bi-O bond is established between CBB and BWO, serving as an "electron bridge". The electrons generated by BWO are efficiently channeled to CBB through the heterojunction-formed "electron bridge", thereby achieving effective photocatalytic CO2 reduction. Under simulated sunlight conditions, it exhibits the highest CO yield of 72.52 mu mol g(-1) (without the addition of any precious metal, photosensitizers or sacrifices), which is approximately 7-fold and 18-fold greater than that of pure CBB and BWO, respectively. This work provides a more profound comprehension of the regulation of electron transfer through interfacial chemical bonds, thereby proposing a promising strategy for the development of efficient heterojunction photocatalysts for CO2 photoreduction.
Keyword :
Bi2WO6 Bi2WO6 CO2 reduction CO2 reduction Perovskite Perovskite Photocatalysis Photocatalysis Z-scheme Z-scheme
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GB/T 7714 | Liu, Haolan , Sun, Jingjing , Lin, Qianying et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction [J]. | CHEMCATCHEM , 2024 , 16 (22) . |
MLA | Liu, Haolan et al. "An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction" . | CHEMCATCHEM 16 . 22 (2024) . |
APA | Liu, Haolan , Sun, Jingjing , Lin, Qianying , Wang, Ying , Wang, Shuo , Wang, Shuowen et al. An Electron Bridge of Shared Atoms Mediated Cs3Bi2Br9/Bi2WO6 Z-Scheme Heterojunction for Photocatalytic CO2 Reduction . | CHEMCATCHEM , 2024 , 16 (22) . |
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Battery-type faradaic materials are considered a class of promising electrodes for capacitive deionization (CDI) due to their superior ability to store ions through redox reactions. However, the desalination potential of such electrode materials has not been fully explored subject to the accessibility, conductivity, stability, etc. Herein, embedded battery material Ag nanoparticles is designed in capsule-structural units composed of graphene and constructed freestanding composite electrodes for CDI. Particularly, these Ag nanoparticles confined in interconnected graphene capsules can be both efficiently accessed by the electrolyte and rationally protected by the capsule networks, significantly unlocking their potential as desalination materials. Impressively, the optimized Ag-involved anodes can achieve an ultrahigh NaCl desalination capacity of approximate to 360 mg g-1 (approximate to 218 mg g-1 for Cl-) at 1.4 V and exhibit good cycling stability. Moreover, the as-designed anodes also have very competitive desalination capacities for other anions, such as SO2- 4 (approximate to 90 mg g-1) and CrO2- 4 (approximate to 77 mg g-1), suggesting the broad applicability of such Ag-involved electrodes. This work shows that the ingenious introduction of space-confined structures is an effective means of unlocking the desalination potential of Ag-based materials, opening up alternative avenues for the development of other high-performance battery-type desalination electrodes.
Keyword :
binder-free binder-free capacitive deionization capacitive deionization capsule structure capsule structure confined redox confined redox faradaic electrodes faradaic electrodes
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GB/T 7714 | Liu, Liyan , You, Shaojie , Liu, Haoyang et al. Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization [J]. | SMALL , 2024 , 21 (1) . |
MLA | Liu, Liyan et al. "Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization" . | SMALL 21 . 1 (2024) . |
APA | Liu, Liyan , You, Shaojie , Liu, Haoyang , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin et al. Battery-Type Desalination Behavior Confined Within Capsules for Efficient Capacitive Deionization . | SMALL , 2024 , 21 (1) . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword :
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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The electrocatalytic conversion of inert CO2 to value-added chemical fuels powered by renewable energy is one of the benchmark approaches to address excessive carbon emissions and achieve carbon-neutral energy restructuring. However, the adsorption/activation of supersymmetric CO2 is facing insurmountable challenges that constrain its industrial-scale applications. Here, this theory-guided study confronts these challenges by leveraging the synergies of bimetallic sites and defect engineering, where pyrochlore-type semiconductor A(2)B(2)O(7) is employed as research platform and the conversion of CO2-to-HCOOH as the model reaction. Specifically, defect engineering intensified greatly the chemisorption-induced CO2 polarization via the bimetallic coordination, thermodynamically beneficial to the HCOOH production via the *HCO2 intermediate. The optimal V-BSO-430 electrocatalyst with abundant surface oxygen vacancies achieved a superior HCOOH yield of 116.7 mmol h(-1) cm(-2) at -1.2 V-RHE, rivalling the incumbent similar reaction systems. Furthermore, the unique catalytic unit featured with a Bi-1-Sn-Bi-2 triangular structure, which is reconstructed by defect engineering, and altered the pathway of CO2 adsorption and activation to allow the preferential affinity of the suspended O atom in *HCO2 to H. As a result, V-BSO-430 gave an impressive FEHCOOH of 93% at -1.0 V-RHE. This study held promises for inspiring the exploration of bimetallic materials from the massive semiconductor database.
Keyword :
A(2)B(2)O(7) A(2)B(2)O(7) bimetallic sites bimetallic sites CO2 reduction CO2 reduction electrocatalysis electrocatalysis pyrochlore pyrochlore
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GB/T 7714 | Zhao, Jiwu , Wang, Jiashun , Xue, Lan et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH [J]. | SMALL , 2024 , 20 (38) . |
MLA | Zhao, Jiwu et al. "Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH" . | SMALL 20 . 38 (2024) . |
APA | Zhao, Jiwu , Wang, Jiashun , Xue, Lan , Wang, Ying , Wen, Na , Huang, Haowei et al. Surface Oxygen Defect Engineering of A2B2O7 Pyrochlore Semiconductors Boosts the Electrocatalytic Reduction of CO2-to-HCOOH . | SMALL , 2024 , 20 (38) . |
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The valorization of native lignin to functionalized aromatic compounds under visible light is appealing yet challenging. In this communication, colloidal mercaptoalkanoic acid capped ultrathin ZnIn2S4 (ZIS) microbelts was successfully fabricated, which was used as a superior catalyst for depolymerization of native lignin in birch woodmeal under visible light, with an optimum yield of 28.8 wt % to functionalized aromatic monomers achieved in 8 h. The capped mercaptoalkanoic acid not only enables a solvent modulated reversible interchange of ZIS between the colloidal state for efficient reaction and the aggregated state for facile separation, but also serves as a precursor for light initiated generation of reactive thiyl radical for highly selective cleavage of beta-O-4 bond in native lignin. This work provides a green and efficient strategy for the depolymerization of native lignin to functionalized aromatic monomers under mild conditions, which involves a new mechanism for the cleavage of beta-O-4 bonds in native lignin. The capability of cleavage of beta-O-4 bonds in native lignin by photogenerated thiyl radicals also demonstrates the great potential of using photogenerated thiyl radicals in organics transformations.
Keyword :
Depolymerization Depolymerization Heterogeneous Catalysis Heterogeneous Catalysis Lignin Lignin Photochemistry Photochemistry Radicals Radicals
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GB/T 7714 | Wang, Jiaqi , Li, Yaxin , Liu, Hurunqing et al. Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
MLA | Wang, Jiaqi et al. "Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 37 (2024) . |
APA | Wang, Jiaqi , Li, Yaxin , Liu, Hurunqing , Ding, Zhengxin , Yuan, Rusheng , Li, Zhaohui . Depolymerization of Native Lignin over Thiol Capped Ultrathin ZnIn2S4 Microbelts Mediated by Photogenerated Thiyl Radical . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (37) . |
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Photocatalytic oxidative coupling of amines is considered a mild, efficient, and sustainable strategy for the synthesis of imines. As a versatile organic semiconductor, conjugated microporous polymers (CMPs) are attractive in photocatalysis areas due to the diversity of their polymeric monomers. Herein, we report that in addition to the design of monomers, size-confined polymerization is also a feasible strategy to modulate the structure and photocatalysis properties of CMPs. We adopted dibromopyrazine as polymeric units to prepare pyrazine-involved hollow spherical CMPs (H-PyB) using a template method and successfully performed sizeconfined polymerization of hollow samples by resizing the templates. Interestingly, the small confinement space induced the formation of CMPs with better conjugate extensibility, resulting in enhanced conductivity, narrowed bandgaps, improved photoelectric performance, etc. As a result, small-sized H-PyB CMPs had superior activity for the photocatalytic oxidation of amines. Particularly, the smallest H-PyB CMPs that we designed in the present work exhibited excellent performance for the photocatalytic coupling oxidation of amines. When using benzylamine as a model substrate, the yield of the corresponding imine reached similar to 113 mmol center dot g(- 1)center dot h(-1), accompanied by almost 100 % selectivity. Furthermore, the as-designed confined samples exhibited stable photocatalytic activity as well as good applicability for oxidative coupling of different amines. This work not merely reports a kind of CMP photocatalysts with excellent performance for the imine coupling oxidation but also proposes an alternative strategy for constructing high-performance organic photocatalysts by size-confined synthesis.
Keyword :
Amine Amine Conjugated microporous polymers Conjugated microporous polymers Photocatalytic oxidation Photocatalytic oxidation Size-confined synthesis Size-confined synthesis Visible light Visible light
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GB/T 7714 | You, Shaojie , Ding, Zhengxin , Yuan, Rusheng et al. Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 664 : 63-73 . |
MLA | You, Shaojie et al. "Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 664 (2024) : 63-73 . |
APA | You, Shaojie , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin , Xu, Chao . Confined synthesis of conjugated microporous polymers for selective photocatalytic oxidation of amines . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 664 , 63-73 . |
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