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学者姓名：龙金林
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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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Metal nanoparticle (NP) cocatalysts are widely investigated for their ability to enhance the performance of photocatalytic materials; however, their practical application is often limited by the inherent instability under light irradiation. This challenge has catalyzed interest in exploring high-entropy alloys (HEAs), which, with their increased entropy and lower Gibbs free energy, provide superior stability. In this study, 3.5 nm-sized noble-metal-free NPs composed of a FeCoNiCuMn HEA are successfully synthesized. With theoretic calculation and experiments, the electronic structure of HEA in augmenting the catalytic CO2 reduction has been uncovered, including the individual roles of each element and the collective synergistic effects. Then, their photocatalytic CO2 reduction capabilities are investigated when immobilized on TiO2. HEA NPs significantly enhance the CO2 photoreduction, achieving a 23-fold increase over pristine TiO2, with CO and CH4 production rates of 235.2 and 19.9 mu mol g(-1) h(-1), respectively. Meanwhile, HEA NPs show excellent stability under simulated solar irradiation, as well high-energy X-ray irradiation. This research emphasizes the promising role of HEA NPs, composed of earth-abundant elements, in revolutionizing the field of photocatalysis.
Keyword ：
high-entropy alloy high-entropy alloy nanoparticle nanoparticle noble-metal-free noble-metal-free photocatalytic CO2 reduction photocatalytic CO2 reduction
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| GB/T 7714 | Huang, Haowei , Zhao, Jiwu , Guo, Hele et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction [J]. | ADVANCED MATERIALS , 2024 , 36 (26) . |
| MLA | Huang, Haowei et al. "Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction" . | ADVANCED MATERIALS 36 . 26 (2024) . |
| APA | Huang, Haowei , Zhao, Jiwu , Guo, Hele , Weng, Bo , Zhang, Hongwen , Saha, Rafikul Ali et al. Noble-Metal-Free High-Entropy Alloy Nanoparticles for Efficient Solar-Driven Photocatalytic CO2 Reduction . | ADVANCED MATERIALS , 2024 , 36 (26) . |
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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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Detoxicating materials of chemical warfare agents (CWAs) and their simulants play a critical role in reducing pollution contamination and environmental renovation. In this work, we present a simple strategy to prepare a core -shell structure Fe 3 O 4 /UiO-66-NH 2 /ILs@mSiO 2 using hydrogen bonding association and electrostatic forces. We performed disinfection studies on dimethyl 4-nitrophenyl phosphate (DMNP) and 2-chloroethyl ethyl sulfide (2-CEES). The synergistic effects of catalytic activations for CWAs, which reduce the electron transport distance and lower the reaction energy barrier, lead to an increase in hydrolysis and Fenton-like reactions efficiency. Eliminationing tests of DMNP and 2-CEES showed that the half-lives of the degradation reactions were 128.36 and 1.12 min, respectively, and the degradation efficiency did not decrease significantly after 4 cycles. This new type of structure could be magnetically separated within 60 s to facilitate material recovery and reuse. Moreover, the presence of a mesoporous silica shell made the catalyst particles to become biocompatible and environmentally friendly. The degradation pathways of the intermediates were revealed based on nuclear magnetic resonance spectroscopy (NMR), gaschromatography-mass spectrometry (GC -MS) and density functional theory (DFT) calculations. The effective combination of catalysts provided a facile strategy for developing multi-effect synergistic catalysts for the elimination of CWAs and other pollutants.
Keyword ：
Biocompatible Biocompatible Chemical Warfare Agents Chemical Warfare Agents Enrichment Capability Enrichment Capability Ionic Liquids Ionic Liquids Metal-Organic Frameworks Metal-Organic Frameworks
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| GB/T 7714 | Zhao, Hua , Li, Yu-Han , Zhao, Hongjie et al. In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
| MLA | Zhao, Hua et al. "In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations" . | SEPARATION AND PURIFICATION TECHNOLOGY 341 (2024) . |
| APA | Zhao, Hua , Li, Yu-Han , Zhao, Hongjie , Wang, Yi , Long, Jinlin , Sun, Ruize et al. In-situ adsorption and detoxification of chemical warfare agent simulants by biocompatible Zr-MOFs immobilized ionic liquids composites: Mechanisms, degradation pathways and DFT calculations . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 341 . |
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Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni-1 SAC on beta-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni-1/beta-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni-1/beta-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
Keyword ：
biomass biomass carbide carbide catalysis catalysis hydrodeoxygenation hydrodeoxygenation single-atom catalyst single-atom catalyst
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| GB/T 7714 | Guo, Haoquan , Zhao, Jiwu , Chen, Yu et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C [J]. | ACS CATALYSIS , 2024 , 14 (2) : 703-717 . |
| MLA | Guo, Haoquan et al. "Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C" . | ACS CATALYSIS 14 . 2 (2024) : 703-717 . |
| APA | Guo, Haoquan , Zhao, Jiwu , Chen, Yu , Lu, Xinyu , Yang, Yue , Ding, Chenrong et al. Mechanistic Insights into Hydrodeoxygenation of Lignin Derivatives over Ni Single Atoms Supported on Mo2C . | ACS CATALYSIS , 2024 , 14 (2) , 703-717 . |
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Wound dressings play a critical role in the wound healing process; however, conventional dressings often address singular functions, lacking versatility in meeting diverse wound healing requirements. Herein, dual-network, multifunctional hydrogels (PSA/CS-GA) have been designed and synthesized through a one-pot approach. The in vitro and in vivo experiments demonstrate that the optimized hydrogels have exceptional antifouling properties, potent antibacterial effects and rapid hemostatic capabilities. Notably, in a full-thickness rat wound model, the hydrogel group displays a remarkable wound healing rate exceeding 95% on day 10, surpassing both the control group and the commercial 3M group. Furthermore, the hydrogels exert an anti-inflammatory effect by reducing inflammatory factors interleukin 6 (IL-6) and tumor necrosis factor-alpha (TNF-alpha), enhance the release of the vascular endothelial growth factor (VEGF) to promote blood vessel proliferation, and augment collagen deposition in the wound, thus effectively accelerating wound healing in vivo. These innovative hydrogels present a novel and highly effective approach to wound healing. Dual network multifunctional hydrogels are developed using a one-pot synthesis approach. The in vitro and in vivo experiments demonstrate that these hydrogels have exceptional antifouling properties, potent antibacterial effects and rapid hemostatic capabilities.
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| GB/T 7714 | Jiang, Hongzhi , Huang, Xueping , Yang, Jiachao et al. Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing [J]. | JOURNAL OF MATERIALS CHEMISTRY B , 2024 , 12 (20) : 4909-4921 . |
| MLA | Jiang, Hongzhi et al. "Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing" . | JOURNAL OF MATERIALS CHEMISTRY B 12 . 20 (2024) : 4909-4921 . |
| APA | Jiang, Hongzhi , Huang, Xueping , Yang, Jiachao , Yu, Xunbin , Yang, Weibo , Song, Yunhao et al. Dual network composite hydrogels with robust antibacterial and antifouling capabilities for efficient wound healing . | JOURNAL OF MATERIALS CHEMISTRY B , 2024 , 12 (20) , 4909-4921 . |
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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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Halogenated methane serves as a universal platform molecule for building high-value chemicals. Utilizing sodium chloride solution for photocatalytic methane chlorination presents an environmentally friendly method for methane conversion. However, competing reactions in gas-solid-liquid systems leads to low efficiency and selectivity in photocatalytic methane chlorination. Here, an in situ method is employed to fabricate a hydrophobic layer of TaOx species on the surface of NaTaO3. Through in-situ XPS and XANES spectra analysis, it is determined that TaOx is a coordination unsaturated species. The TaOx species transforms the surface properties from the inherent hydrophilicity of NaTaO3 to the hydrophobicity of TaOx/NaTaO3, which enhances the accessibility of CH4 for adsorption and activation, and thus promotes the methane chlorination reaction within the gas-liquid-solid three-phase system. The optimized TaOx/NaTaO3 photocatalyst has a good durability for multiple cycles of methane chlorination reactions, yielding CH3Cl at a rate of 233 mu mol g(-1) h(-1) with a selectivity of 83%. In contrast, pure NaTaO3 exhibits almost no activity toward CH3Cl formation, instead catalyzing the over-oxidation of CH4 into CO2. Notably, the activity of the optimized TaOx/NaTaO3 photocatalyst surpasses that of reported noble metal photocatalysts. This research offers an effective strategy for enhancing the selectivity of photocatalytic methane chlorination using inorganic chlorine ions.
Keyword ：
hydrophobicity hydrophobicity methane chlorination methane chlorination photocatalysis photocatalysis TaOx TaOx ultrathin layer ultrathin layer
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| GB/T 7714 | Li, Dongmiao , Lin, Min , Zhang, Jiangjie et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Li, Dongmiao et al. "Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine" . | SMALL 20 . 38 (2024) . |
| APA | Li, Dongmiao , Lin, Min , Zhang, Jiangjie , Qiu, Chengwei , Chen, Hui , Xiao, Zhen et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine . | SMALL , 2024 , 20 (38) . |
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Bacterial infections are a major public health challenge around the world. The development of novel surface coatings that effectively inhibit bacterial adhesion, proliferation and growth is a critical step in addressing this global challenge. Photocatalytic antibacterial therapy has proven to be an effective approach and has received increasing attention. However, it is still a challenge to obtain coatings with both antibacterial adhesion and durable photocatalytic antibacterial functions. Herein, an acridine-based coating with antibacterial adhesion and photocatalytic antibacterial properties was prepared by simple methods (i.e., spin-coating, spray-coating, and drop-coating) and can be applied to various substrates. The bacterial anti-adhesion test results showed that the coating could effectively prevents the adhesion of Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), and Pseudomonas aeruginosa (P. aeruginosa), indicating the strong anti-fouling capability. The acridine-based coating demonstrated durable photocatalytic antimicrobial activity, remaining 99.3 % antibacterial effective against all three bacterial strains even after 30 days exposed to visible light. The coating can significantly reduce or eliminate the risk of contamination and cross-contamination, making it ideal for use in public healthcare environments. © 2024
Keyword ：
Adhesion Adhesion Coatings Coatings Contamination Contamination Escherichia coli Escherichia coli Photocatalytic activity Photocatalytic activity
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| GB/T 7714 | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial [J]. | Progress in Organic Coatings , 2024 , 194 . |
| MLA | Kang, Linfeng et al. "Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial" . | Progress in Organic Coatings 194 (2024) . |
| APA | Kang, Linfeng , Peng, Houqian , Yang, Mingyuan , Hu, Ke , Lin, Yihui , Zhu, Yongchao et al. Dual-functional acridine-based coatings with anti-bacterial adhesion and durable photocatalytic antibacterial . | Progress in Organic Coatings , 2024 , 194 . |
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