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学者姓名：梁诗景
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Abstract ：
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N-2 in aqueous solution, the high dissociation energy of N equivalent to N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO(2 )achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at -0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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| GB/T 7714 | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction [J]. | LANGMUIR , 2024 , 40 (10) : 5469-5478 . |
| MLA | Sun, Zhuangzhi et al. "Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction" . | LANGMUIR 40 . 10 (2024) : 5469-5478 . |
| APA | Sun, Zhuangzhi , Lin, Jiawei , Lu, Suwei , Li, Yuhang , Qi, Tingting , Peng, Xiaobo et al. Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction . | LANGMUIR , 2024 , 40 (10) , 5469-5478 . |
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Reasonable adjustment of the exposed crystal facets has been proven to be an effective strategy to improve the activity of the catalyst. However, the crystal-facet-dependent piezoactivity is rarely investigated. In this work, BiFeO3 with highly exposed (012) or (110) crystal facets were synthesized by adjusting the volume ratio of solvent and reaction time. Ethylene glycol was used as a structure-directing agent for the synthesis of BiFeO3 nanosheets (BiFeO3-NS) with highly exposed (012) facets. BiFeO3-NS shows an obvious higher piezoelectric catalytic hydrogen evolution rate than that of BiFeO3 nanoparticles (BiFeO3-NP) with highly exposed (110) facets. In addition, the rate constant of BiFeO3-NS for the piezocatalytic degradation of rhodamine B (RhB) shows a 2-fold increase than that of BiFeO3-NP. A variety of controlled experiments have been performed. It is revealed that these two nanomaterials exhibit comparable specific surface areas and adsorption capacity. BiFeO3-NS possesses narrowed bandgap as compared to that of BiFeO3-NP. The enhanced piezocatalytic activity of BiFeO3-NS can be attributed to its built-in electric field, strong carrier mobility, and effective charge separation efficiency. This study provides an alternative perspective for piezoelectric catalysis in surface engineering.
Keyword ：
BiFeO3 BiFeO3 crystal facets crystal facets dye degradation dye degradation hydrogenevolution hydrogenevolution piezocatalysis piezocatalysis
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| GB/T 7714 | Wang, Xiangge , Lu, Xiaoxiao , Zhao, Xiaojing et al. Crystal-Facet-Dependent Piezocatalytic Activity of BiFeO3 Nanosheets for H2 Evolution and Environmental Remediation [J]. | ACS APPLIED NANO MATERIALS , 2024 , 7 (10) : 11794-11802 . |
| MLA | Wang, Xiangge et al. "Crystal-Facet-Dependent Piezocatalytic Activity of BiFeO3 Nanosheets for H2 Evolution and Environmental Remediation" . | ACS APPLIED NANO MATERIALS 7 . 10 (2024) : 11794-11802 . |
| APA | Wang, Xiangge , Lu, Xiaoxiao , Zhao, Xiaojing , Chen, Wen-Jie , Liu, Yubin , Pan, Xiaoyang et al. Crystal-Facet-Dependent Piezocatalytic Activity of BiFeO3 Nanosheets for H2 Evolution and Environmental Remediation . | ACS APPLIED NANO MATERIALS , 2024 , 7 (10) , 11794-11802 . |
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Photocatalytic N2 reduction using H2O to produce NH3 offers a promising alternative to the energy-intensive Haber-Bosch process. Nevertheless, its efficiency is hampered by the low solubility of N2 in water, the high stability of N---N and the competing H2 evolution reaction (HER). In this study, we present a highly efficient nanohybrid system employing BiOBr nanoflowers with O defect as a platform for anchoring Ru. The designed nanohybrids exhibit a significantly higher NH3 generation rate of 121.97 mu mol g-1 h-1, which is 6.1 and 2.8 times higher than that of pristine BiOBr-NS and Ru modified BiOBr without O defect, respectively. Experimental analyses and theoretical calculations reveal that the nanoflower structure with confined nano-space promotes the enrichment of N2 on the catalyst, the synergistic O defects and Ru facilitate the selective adsorption and activation of N2 and lower the energy barriers of the rate-determining *N-N to *N-NH step.
Keyword ：
BiOBr BiOBr Confined structure Confined structure N 2 reduction N 2 reduction Photocatalysis Photocatalysis Synergistic active units Synergistic active units
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| GB/T 7714 | Xia, Yuzhou , Xia, Xinghe , Chen, Lu et al. O defect anchored Ru on BiOBr with nanoconfined structure for catalytic N2 fixation [J]. | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 349 . |
| MLA | Xia, Yuzhou et al. "O defect anchored Ru on BiOBr with nanoconfined structure for catalytic N2 fixation" . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY 349 (2024) . |
| APA | Xia, Yuzhou , Xia, Xinghe , Chen, Lu , Liang, Ruowen , Yan, Guiyang , Liang, Shijing . O defect anchored Ru on BiOBr with nanoconfined structure for catalytic N2 fixation . | APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY , 2024 , 349 . |
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Simultaneous H2 production and benzyl alcohol oxidation is an effective strategy for fully utilizing photoexcited electrons and holes of the photocatalysts. Herein, PtO are decorated on hollow CdS microspheres to fabricate a coupling photocatalytic system for accelerating H2 generation and selective oxidation of benzyl alcohol to benzaldehyde. The PtO-CdS hollow microspheres have been prepared by a facile hydrothermal method without any template agents. Under simulated sunlight irradiation, the 1 %PtO/CdS exhibited the highest rates of H2 evolution and benzaldehyde production. In addition, the PtO-CdS photoctalyst is stable during five cycles of photocatalytic reaction. Photoelectrochemical analyses coupled with ESR measurement demonstrated that PtO decoration not only promotes the charge separation but also improves the stability of the CdS. It is hoped that this work would provide useful information for the synthesis of CdS nanostructure for target application.
Keyword ：
CdS CdS Composite materials Composite materials H 2 production H 2 production Selective oxidation Selective oxidation Solar energy materials Solar energy materials
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| GB/T 7714 | Wang, Xiangge , Huang, Mianli , Xu, Miaoqiong et al. Hydrogen production coupled with benzyl alcohol oxidation promoted by PtO-CdS hollow microsphere photocatalysts [J]. | MATERIALS LETTERS , 2024 , 361 . |
| MLA | Wang, Xiangge et al. "Hydrogen production coupled with benzyl alcohol oxidation promoted by PtO-CdS hollow microsphere photocatalysts" . | MATERIALS LETTERS 361 (2024) . |
| APA | Wang, Xiangge , Huang, Mianli , Xu, Miaoqiong , Pan, Xiaoyang , Liang, Shijing . Hydrogen production coupled with benzyl alcohol oxidation promoted by PtO-CdS hollow microsphere photocatalysts . | MATERIALS LETTERS , 2024 , 361 . |
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Ordered mesoporous carbon@silica hybrid frameworks with high nitrogen content and good stabilities show great significance to improve their functionalities. Herein, we report novel nitrogen-doped (3.51 - 4.62 wt%) and ordered mesoporous carbon@silica frameworks (N-OMC@SiO2) with reinforced nitrogen stability. The NOMC@SiO2 were designed from tricomponent direct co-assembly between block copolymer template and mixed precursors containing urea and tetramethoxysilane without using additional solvent. The N-OMC@SiO2 have large BET surface areas (444.3 - 674.9 m2/g), uniform mesoporous channels (5.8 - 10.9 nm) with well-defined hexagonal symmetry, and stable carbon@silica "reinforced concrete" framework that can be transformed into carbon@silicon by controllable reduction. The nitrogen sites were firmly embedded into their frameworks via the formation of Si-N bonding. Thus, the resulted N-OMC@SiO2 exhibit multi-functionalities and enhanced recyclability in acid waste gas capture and gaseous sulfides catalytic utilization, better than many reported porous adsorbents and catalysts. This study may help develop stable and efficient N-OMCs nanocomposites for acidic gas selective removal.
Keyword ：
Acid gas selective capture Acid gas selective capture Carbon@silica composites Carbon@silica composites Gaseous sulfides elimination Gaseous sulfides elimination Nitrogen -doping Nitrogen -doping Ordered mesoporosity Ordered mesoporosity Solvent -free synthesis Solvent -free synthesis
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| GB/T 7714 | Kan, Xun , Liu, Zihao , Sun, Yafei et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
| MLA | Kan, Xun et al. "Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities" . | CHEMICAL ENGINEERING SCIENCE 292 (2024) . |
| APA | Kan, Xun , Liu, Zihao , Sun, Yafei , Zhong, Shouchao , Zheng, Yong , Liang, Shijing et al. Tricomponent direct co-assembly to nitrogen-doped, ordered mesoporous carbon@silica frameworks with enhanced nitrogen stability and multi-functionalities . | CHEMICAL ENGINEERING SCIENCE , 2024 , 292 . |
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Electrocatalytic nitrogen (N2) reduction to ammonia (NH3) reaction (eNRR) supplies a promising alternative to the Haber-Bosch technology. However, the dissociation of N[tbnd]N bond hinders its development. Herein, sulfur vacancies are introduced into FeS2 for promoting N2 activation and thus stimulating the eNRR progress. Experimental investigations and density functional theory (DFT) calculations reveal that the electrons could transfer from Fe 3d orbits to N2 2π* orbital, thus facilitating the cracking of inert N2 molecules. And the electron transfer is easier for those Fe atoms with S vacancies in adjacent positions. Furthermore, we find that eNRR process on the FeS2 surface follows the distal and alternating hybrid pathway. Also, the water molecules in the electrolyte facilitate the first hydrogenation of N2 (*N2 → *NNH). Notably, FeS2 with rich sulfur vacancies exhibits an excellent NH3 yield rate of 67.5 μg h−1 mgcat.−1, which outperforms most of the reported eNRR activities of Fe-based catalysts. © 2024
Keyword ：
Density functional theory Density functional theory Electrocatalytic nitrogen reduction Electrocatalytic nitrogen reduction N2 activation N2 activation Sulfur defect Sulfur defect
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| GB/T 7714 | Lin, J. , Lin, X. , Lu, S. et al. Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia [J]. | Chemical Engineering Science , 2024 , 300 . |
| MLA | Lin, J. et al. "Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia" . | Chemical Engineering Science 300 (2024) . |
| APA | Lin, J. , Lin, X. , Lu, S. , Liao, W. , Qi, T. , Liang, S. et al. Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia . | Chemical Engineering Science , 2024 , 300 . |
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Lignin, characterized by its amorphous, heavily polymerized structure, is a primary natural source of aromatic compounds, yet its complex constitution poses considerable challenges in its transformation and utilization. Therefore, the selective cleavage of C-C bonds represents a critical and challenging step in lignin degradation, essential for the production of high-value aromatic compounds. In this study, we report a simple electrocatalytic approach for lignin valorization via C-C bond cleavage by developing a nonmetallic electrocatalyst of carbon-based materials. It is found that the hydrophilicity and hydrophobicity of the electrocatalyst have a significant effect on the degradation process. Under mild conditions, the hydrophilic carbon paper exhibits 100% substrate conversion, yielding 97% benzaldehyde and 96% quinone with ionic liquid electrolytes. The mechanism study shows that the carbon catalyst with higher surface defects favors electron transfer in the oxidative cleavage process of C-C bonds. These results signify a substantial advancement in lignin degradation, offering an environmentally friendly, metal-free electrochemical route. © 2024 The Authors. Co-published by Zhejiang University and American Chemical Society.
Keyword ：
Amorphous carbon Amorphous carbon Aromatization Aromatization Covalent bonds Covalent bonds Electrolytes Electrolytes Quinone Quinone
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| GB/T 7714 | Liu, Guangyong , Zhai, Ziqi , Lu, Yumiao et al. Electrocatalytic Cleavage of C-C Bonds in Lignin Models Using Nonmetallic Catalysts at Ambient Conditions [J]. | Chem and Bio Engineering , 2024 , 1 (4) : 357-365 . |
| MLA | Liu, Guangyong et al. "Electrocatalytic Cleavage of C-C Bonds in Lignin Models Using Nonmetallic Catalysts at Ambient Conditions" . | Chem and Bio Engineering 1 . 4 (2024) : 357-365 . |
| APA | Liu, Guangyong , Zhai, Ziqi , Lu, Yumiao , Lu, JunFeng , Wang, Yanlei , Liang, Shijing et al. Electrocatalytic Cleavage of C-C Bonds in Lignin Models Using Nonmetallic Catalysts at Ambient Conditions . | Chem and Bio Engineering , 2024 , 1 (4) , 357-365 . |
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The catalytic cleavage of carbon-sulfur (C & boxH;S) double bonds on the metal sites without deactivation has aroused great interest in both fundamental catalytic research and industrial chemistry. Herein, activity descriptors are developed via machine learning and density functional theory (DFT) calculations to screen transition-metal single-site catalysts, which quantify the effect of both atomic electronic properties and coordination configuration on the hydrolysis of C & boxH;S double bonds. The valence electron number and electronegativity of active sites are found to be well related to C & boxH;S activation and sulfur poisoning, where Fe demonstrates high catalytic potential among a series of metal centers. On the other hand, the isolated Fe-1 and Fe-2 sites favor carbonyl sulfide (COS) adsorption and activation, while the COS easily dissociates into *S and *CO on Fe-3 hollow site, thus resulting in the formation of robust Fe-S bonds and catalyst deactivation. As anticipated, the as-designed Fe-1-N-4 site achieves a COS conversion of ca. 96% at 100 degrees C, slightly better than the Fe-2-N-4 site, approximately 8 times higher than that of the Fe/C, which is also better than those of other monatomic catalysts (such as Co-NC, Ni-NC, Sn-NC, and Bi-NC). The combination of in situ characterizations and theoretical calculations suggests that *COS and *H2O/*OH have a competitive adsorption relationship on Fe-N-4 sites, and two Fe-N-4 sites can synergistically catalyze the COS hydrolysis through the spilled H and OH.
Keyword ：
carbon-sulfurbonds cleavage carbon-sulfurbonds cleavage hydrolysis mechanism exploration hydrolysis mechanism exploration isolated Fe-N-4 site isolated Fe-N-4 site metal activesite design metal activesite design valence electron descriptor valence electron descriptor
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| GB/T 7714 | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds [J]. | ACS CATALYSIS , 2024 , 14 (22) : 17103-17112 . |
| MLA | Lei, Ganchang et al. "Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds" . | ACS CATALYSIS 14 . 22 (2024) : 17103-17112 . |
| APA | Lei, Ganchang , Lin, Xiaoyun , Yan, Hongping , Shen, Lijuan , Wang, Shiping , Liang, Shijing et al. Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon-Sulfide Double Bonds . | ACS CATALYSIS , 2024 , 14 (22) , 17103-17112 . |
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In this work, 44 metal-organic frameworks (MOFs) are screened for efficient electrocatalytic nitrogen reduction reaction (eNRR). The isosteric heats of N2 adsorption on the 44 metal active centers of MOFs are calculated by the grand canonical Monte Carlo method. It is found that p-block-elements exhibit the highest N2 affinity among all screened elements, implying their excellent catalytic potentials for eNRR. Furthermore, the Al element is preferentially chosen as the metal center of MOFs (MIL-53 (Al)) owing to its relatively low toxicity and cost. Combined in situ Diffuse Reflectance Infrared Fourier Transform (DRIFT) analysis with theoretical calculation, we found that N2 is mainly attracted by the bridging oxygen of Al-O-Al structure in the MIL-53 (Al). The optimized MIL-53 (Al) shows a superior activity with the NH3 yield rate of 74.55 +/- 1 mu g h-1 mgcat-1 at -0.3 V vs. Reversible Hydrogen Electrode (RHE), to our best knowledge, which is currently the highest activity of MOF-based catalyst for eNRR reported in the literature.
Keyword ：
electrocatalytic nitrogen reduction reaction electrocatalytic nitrogen reduction reaction metal-organic framework metal-organic framework MIL-53 (Al) MIL-53 (Al) screening screening
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| GB/T 7714 | Lin, Jiawei , Li, Yuhang , Yan, Hongping et al. Screening of metal-organic frameworks for efficient electrocatalytic nitrogen reduction [J]. | AICHE JOURNAL , 2024 , 71 (3) . |
| MLA | Lin, Jiawei et al. "Screening of metal-organic frameworks for efficient electrocatalytic nitrogen reduction" . | AICHE JOURNAL 71 . 3 (2024) . |
| APA | Lin, Jiawei , Li, Yuhang , Yan, Hongping , Qi, Tingting , Liang, Shijing , Jiang, Lilong . Screening of metal-organic frameworks for efficient electrocatalytic nitrogen reduction . | AICHE JOURNAL , 2024 , 71 (3) . |
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Electrocatalytic depolymerization of lignin into value-added chemicals offers a promising technique to make biorefining sustainable.Herein,we report a robust trimetallic PdNiBi electrocatalyst for reductive C-O bond cleavage of different lignin model dimers and oxidized lignin under mild conditions.The reduction reaction proceeds with complete substrate conversion and excellent yields toward monomers of phenols(80％-99％)and acetophenones(75％-96％)in the presence of an ionic liquid electrolyte with operational stability.Systematic experimental investigations together with density functional theory(DFT)calculations reveal that the outstanding performance of the catalyst results from the synergistic effect of the metal elements,which facilitates the easier formation of a key Cα radical intermediate and the facile desorption of the as-formed products at the electrode.The results open up new opportunities for lignin valorization through the green electrocatalytic approach.
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| GB/T 7714 | Guangyong Liu , Yumiao Lu , JunFeng Lu et al. Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions [J]. | 纳米研究（英文版） , 2024 , 17 (4) : 2420-2428 . |
| MLA | Guangyong Liu et al. "Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions" . | 纳米研究（英文版） 17 . 4 (2024) : 2420-2428 . |
| APA | Guangyong Liu , Yumiao Lu , JunFeng Lu , Yanlei Wang , Shijing Liang , Hongyan He et al. Ionic liquid-trimetallic electrocatalytic system for C-O bond cleavage in lignin model compounds and lignin under ambient conditions . | 纳米研究（英文版） , 2024 , 17 (4) , 2420-2428 . |
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