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学者姓名：员汝胜
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Abstract ：
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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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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Prussian blue analogues (PBAs) have been widely studied as cathodes for potassium-ion batteries (PIBs) due to their three-dimensional framework structure and easily adjustable composition. However, the phase transition behavior and [Fe(CN)(6)](4-) anionic defects severely deteriorate electrochemical performances. Herein, we propose a defect-free potassium iron manganese hexacyanoferrate (K1.47Fe0.5Mn0.5[Fe(CN)(6)]1.26H(2)O, KFMHCF-1/2) as the cathode material for PIBs. The Fe-Mn binary synergistic and defect-free effects can inhibit the cell volume change and octahedral slip during the K-ion insertion/extraction process, so that the phase transformation behavior (monoclinic <-> cubic) is effectively inhibited, achieving a zero-strain solid solution mechanism employing Fe and Mn as dual active-sites. Thus, KFMHCF-1/2 contributes the highest initial capacity of 155.3 mAhg(-1) with an energy density of 599.5 Whkg(-1) at 10 mAg(-1) among the reported PBA cathodes, superior rate capability, and cyclic stability over 450 cycles. The assembled K-ion full battery using K deposited on graphite (K@G) as anode also delivers high reversible specific capacity of 131.1 mAhg(-1) at 20 mAg(-1) and ultralong lifespans over 1000 cycles at 50 mAg(-1) with the lowest capacity decay rate of 0.044% per cycle. This work will promote the rapid application of high-energy-density PIBs.
Keyword ：
ammonia synthesis ammonia synthesis flow-throughelectrode flow-throughelectrode lamellar electrified membrane lamellar electrified membrane MXene MXene nitrate reduction nitrate reduction sustainable operation sustainable operation
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| GB/T 7714 | Yang, Xin , Wei, Guanbao , Cao, Jihui et al. Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (8) : 3378-3389 . |
| MLA | Yang, Xin et al. "Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12 . 8 (2024) : 3378-3389 . |
| APA | Yang, Xin , Wei, Guanbao , Cao, Jihui , Ding, Zhengxin , Yuan, Rusheng , Long, Jinlin et al. Mxene-Cu Electrified Membranes with Confined Lamellar Channels for the Flow-through Electrochemical Reduction of Nitrate to Ammonia . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (8) , 3378-3389 . |
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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 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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CdS/UiO-66-NH2 nanocomposite was solvothermally fabricated from cadmium acetate and the pre -synthesized UiO-66-NH2 in dimethyl sulfoxide (DMSO), which acted as the sulfur source. The as -obtained CdS/UiO-66-NH2 nanocomposite was immobilized on a glass fiber cloth (GF) and was applied for hydrogen sulfide (H2S) removal. The resultant GF immobilized CdS/UiO-66-NH2 nanocomposite exhibited a superior activity and high stability for H2S removal under visible light, in which UiO-66-NH2 acts as the main adsorbent and enriches H2S to promote CdS-based photocatalysis, while photocatalysis by CdS decomposes H2S adsorbed on UiO-66-NH2 to realize an in -situ regeneration of the adsorbent. The introduction of UiO-66-NH2 as the main adsorbent suppresses a fast deactivation of CdS due to an irreversible coordination between metal cation Cd2+ and H2S. This study not only developed a new type of material for fast and efficient removal of H2S, but also underscores the high potential of coupling physical adsorption and photocatalysis for the removal of volatile organic compounds (VOCs) and other gaseous pollutants in the environment.
Keyword ：
Adsorption Adsorption CdS CdS Hydrogen sulfide Hydrogen sulfide Photocatalysis Photocatalysis UiO-66-NH 2 UiO-66-NH 2
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| GB/T 7714 | Bai, Yaohui , Chen, Honghan , Cheng, Hao et al. Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
| MLA | Bai, Yaohui et al. "Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide" . | SEPARATION AND PURIFICATION TECHNOLOGY 341 (2024) . |
| APA | Bai, Yaohui , Chen, Honghan , Cheng, Hao , Ding, Zhengxin , Yuan, Rusheng , Li, Zhaohui . Coupling physical adsorption and photocatalysis over CdS/UiO-66-NH2 for efficient removal of hydrogen sulfide . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
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Photothermal catalytic N-acetylation of aniline has been a promising strategy to synthesize amides, which combined the advantages of thermal catalysis and photocatalysis. Herein, we demonstrate a high-performance strategy to synthesize amides catalyzed by the in-situ formed first-row transition-metal (Fe, Co, Ni, Mn et al.) complexes nanodots (TMC NDs) under solar light excitation without using noble metals or strong acids. The dualfunctional nitriles substrates acted as the ligands to coordinate with transition-metal salts affording photosensitive TMC NDs with high solar-to-thermal energy conversion efficiency. Intramolecular charge transitions reduced the energy barrier of nitriles activation by weakening C---N bond and triggered near-field temperature rise via the electron-phonon scattering non-radiative pathway. The reaction system exhibited good tolerance to different functional groups, affording a series of amide derivatives. Such a dynamic coordination reaction mode and the in-situ formed TMC NDs opens new avenues toward solar-heat conversion via photon-phonon coupling in the field of chemical synthesis.
Keyword ：
Amide synthesis Amide synthesis N-acyl sources N-acyl sources Photon -phonon coupling Photon -phonon coupling Photothermal catalysis Photothermal catalysis Transition-metal complexes nanodots Transition-metal complexes nanodots
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| GB/T 7714 | Ma, Xiong-Feng , Xiao, Rui , Wei, Yingcong et al. Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 344 . |
| MLA | Ma, Xiong-Feng et al. "Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 344 (2024) . |
| APA | Ma, Xiong-Feng , Xiao, Rui , Wei, Yingcong , Zhang, Shaohui , Hu, Xiaoyi , Zhang, Ling et al. Photothermal catalytic conversion of water and inert nitriles to amide activated by in-situ formed transition-metal-complex nanodots . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 344 . |
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The integration of electrochemical CO2 reduction (CO2RR) and photoelectrochemical water oxidation offers a sustainable access to valuable chemicals and fuels. Here, we develop a rapidly annealed hematite photoanode with a photocurrent density of 2.83 mA cm-2 at 1.7 VRHE to drive the full-reaction. We also present Cu-alloys electrocatalysis extended from CuInSnS4, which are superior in both activity and selec-tivity for CO2RR. Specifically, the screened CuInSn achieves a CO2 to HCOOH Faradaic efficiency of 93% at a cell voltage of-2.0 V by assembling into artificial photosynthesis cell. The stability test of IT exhibits less than 3% degradation over 24 h. Furthermore, in-situ Raman spectroscopy reveals that both CO2-3 and CO2 are involved in CO2RR as reactants. The preferential affinity of C for H in the *HCO2 intermediate enables an improved HCOOH-selectivity, highlighting the role of multifunctional Cu in reducing the cell voltage and enhancing the photocurrent density.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
Keyword ：
CO2 reduction CO2 reduction CuInSnS4 CuInSnS4 In-situ spectroscopy In-situ spectroscopy Rapid annealing Rapid annealing
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| GB/T 7714 | Zhao, Jiwu , Huang, Liang , Xue, Lan et al. Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells [J]. | JOURNAL OF ENERGY CHEMISTRY , 2023 , 79 : 601-610 . |
| MLA | Zhao, Jiwu et al. "Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells" . | JOURNAL OF ENERGY CHEMISTRY 79 (2023) : 601-610 . |
| APA | Zhao, Jiwu , Huang, Liang , Xue, Lan , Niu, Zhenjie , Zhang, Zizhong , Ding, Zhengxin et al. Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells . | JOURNAL OF ENERGY CHEMISTRY , 2023 , 79 , 601-610 . |
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The electrocatalytic conversion of CO2 waste into liquid fuels is one of the most promising approaches to contribute to carbon neutrality and sustainable energy cycles. Designing and screening efficient electrocatalysts to simultaneously reduce the overpotential required for the CO2 reduction reaction (CO2RR), enhancing product selectivity and current density, still remains challenging. The high concentration of S vacancies in sulfides that can serve as active sites offers the possibility to address these challenges. Here, this study deciphers the positive roles of S vacancies in boosting the adsorption and activation of CO2 by modulating the local electronic structure through theoretical simulations on the In4SnS8 platform. The comparison experiments confirm that sulfides with a high concentration of intrinsic S vacancies are more competitive in selectivity and activity. Afterward, the post-processing heating desulfurization method is employed to create more abundant artificial S vacancies to further verify its effectiveness. The HCOOH Faradaic efficiency (FE) of the post-processed V-In4SnS8-350 with both intrinsic and artificial S vacancies is as high as 91%, which is much higher than 65% for pristine In4SnS8 with only intrinsic S vacancies. Meanwhile, the abundant artificial S vacancies not only upgrade the HCOOH yield from 2.2 to 14.0 mmol center dot h-1 center dot cm-2 but also optimize the bias potential with the highest FE from -1.3 to -1.0 VRHE. These results highlight the effectiveness triggered by intrinsic and artificial S vacancies in enhancing the current density and lowering the optimal bias potential window, as well as improving the HCOOH selectivity. This work not only provides a sound guideline for the development of advanced sulfide semiconductor electrocatalysts but also renders insightful information on multifunctional S vacancies in the CO2RR.
Keyword ：
CO2RR CO2RR HCOOH HCOOH In4SnS8 In4SnS8 sulfide semiconductors sulfide semiconductors sulfur vacancy defects sulfur vacancy defects
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| GB/T 7714 | Niu, Zhenjie , Gao, Xin , Lou, Shuyun et al. Theory-Guided S-Defects Boost Selective Conversion of CO2 to HCOOH over In4SnS8 Nanoflowers [J]. | ACS CATALYSIS , 2023 : 2998-3006 . |
| MLA | Niu, Zhenjie et al. "Theory-Guided S-Defects Boost Selective Conversion of CO2 to HCOOH over In4SnS8 Nanoflowers" . | ACS CATALYSIS (2023) : 2998-3006 . |
| APA | Niu, Zhenjie , Gao, Xin , Lou, Shuyun , Wen, Na , Zhao, Jiwu , Zhang, Zizhong et al. Theory-Guided S-Defects Boost Selective Conversion of CO2 to HCOOH over In4SnS8 Nanoflowers . | ACS CATALYSIS , 2023 , 2998-3006 . |
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