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学者姓名：梁诗景
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Abstract ：
The identification of novel and efficient piezoelectric catalysts is crucial for practical applications. Utilizing Density Functional Theory (DFT) calculations, ZnIn2S4 (ZIS), possessing a non-central symmetric crystal structure, is identified as a promising piezoelectric material for piezocatalysis. Hierarchical ZIS nanosheets are synthesized through a facile hydrothermal method, and defect engineering is employed to enhance their activity. By optimizing the defect concentration, ZIS-300, with the optimal defect level, demonstrates the highest H2 production rate of approximately 3164.67 mu mo1.g- 1.h- 1 under ultrasound, surpassing previously reported piezocatalysts. Furthermore, ZIS-300 exhibits good stability, maintaining its activity and structural integrity after five cycles. Detailed piezo-electrochemical analyses attribute the enhanced piezocatalytic performance to the introduction of sulfur vacancies, which create a shallow donor band facilitating the generation and separation of charge carrier. This work contributes to a deeper understanding of designing high-performance piezocatalysts through theoretical calculations and defect engineering strategies.
Keyword ：
Defect Defect Piezocatalyst Piezocatalyst Sulfur vacancy Sulfur vacancy
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| GB/T 7714 | Huang, Mianli , Zhang, Hongli , Xu, Miaoqiong et al. Controllable engineering of ZnIn2S4 with sulfur vacancy as an efficient piezocatalyst toward H2 production [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2025 , 1016 . |
| MLA | Huang, Mianli et al. "Controllable engineering of ZnIn2S4 with sulfur vacancy as an efficient piezocatalyst toward H2 production" . | JOURNAL OF ALLOYS AND COMPOUNDS 1016 (2025) . |
| APA | Huang, Mianli , Zhang, Hongli , Xu, Miaoqiong , Chen, Wen-Jie , Pan, Xiaoyang , Liang, Shijing . Controllable engineering of ZnIn2S4 with sulfur vacancy as an efficient piezocatalyst toward H2 production . | JOURNAL OF ALLOYS AND COMPOUNDS , 2025 , 1016 . |
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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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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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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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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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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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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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面向国家绿色低碳战略目标,变革化石资源合成氨技术路线变得尤为迫切,开发可再生能源制"绿氨"将成为合成氨领域未来的重要发展方向.将工业废水中的硝酸根(NO3-)电催化还原为氨(NO3RR),既可有效回收氨,又能消除硝酸根污染影响.然而,NO3RR涉及缓慢的八电子转移过程,含有多种反应中间体,其反应机理复杂不明.此外,水系电解液中存在的析氢竞争反应也为高效NO3RR催化剂的开发设计带来了巨大的挑战.为突破高效催化剂的发展瓶颈,本文通过理论模拟,在低成本的催化剂上设计了高效的NO3RR催化活性位点,并利用简单的制备策略合成了目标催化剂.同时,结合原位表征技术,阐明了 NO3RR的反应路径及催化机理. 本文通过密度泛函理论(DFT)计算发现,Cu/TiO2催化剂上的Cu-O-Ti-Ov结构具有较好的NO3-还原活性,该结构不仅能够促进反应中间体NOx-的吸附和活化,还能有效抑制竞争析氢反应,从而降低NO3RR的反应能垒.在该结构上,NO3RR的反应路径为:NO3*→NO2*→ HONO*→ NO*→*NOH →*N →*NH →*NH2 →*NH3→NH3.基于理论计算结果,分别采用浸渍法和尿素水解法制备了系列富含Cu-O-Ti-Ov结构的Cu/TiO2催化剂.氮气等温吸附-脱附曲线、拉曼光谱(Raman)、电子顺磁共振波谱、X射线光电子能谱(XPS)和傅立叶红外光谱等结果发现,相比于采用浸渍法制备的系列Cu/TiO2催化剂,采用尿素水解法制备的Cu/TiO2(CT-U)催化剂具有更大的比表面积以及更多的Cu-O-Ti-Ov位点,说明尿素水解法可提高Cu颗粒在TiO2载体表面的分散度,增强Cu颗粒与TiO2载体之间的相互作用,提高Cu/TiO2催化剂表面的Cu-O-Ti-Ov位点含量.将以上制备出的催化剂应用于催化NO3RR中,结果表明,在-1.0 V vs.RHE还原电位下,CT-U催化剂上氨产率可达3046.5μg h-1 mgcat-1,高于大多数文献报道结果.循环稳定性测试结果表明,在Cu/TiO2催化剂上构建Cu-O-Ti-Ov位点还能显著抑制电催化反应过程中Cu物种从Cu/TiO2催化剂上溶出,从而显著增强催化剂的稳定性.此外,设计制备了不含氧空位的Cu/TiO2,TiO2-x,Cu,Cu2O以及CuO催化剂,并将其用于催化NO3RR.结果发现,上述催化剂上的氨产率皆明显低于CT-U催化剂,说明Cu,Ti以及Ov构成的Cu-O-Ti-Ov结构具有较好的催化协同作用,从而显著提升了NO3RR反应活性.最后,通过原位Raman及原位XPS表征检测反应中间体,验证了由DFT模拟出的NO3RR反应路径. 综上,通过在Cu/TiO2催化剂上理论指导构建Cu-O-Ti-Ov活性位点,实现了NO3RR性能的有效提升.Cu-O-Ti-Ov结构中的多位点协同作用不仅促进了 NOx-的吸附和活化,而且抑制了电催化过程中Cu物种从催化剂上的溶出,从而提高了催化剂的稳定性.本研究为设计高效稳定的NO3RR催化剂提供了新思路.
Keyword ：
Cu-O-Ti-Ov位点 Cu-O-Ti-Ov位点 Cu/TiO2催化剂 Cu/TiO2催化剂 协同催化 协同催化 合成氨 合成氨 电催化硝酸盐还原 电催化硝酸盐还原
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| GB/T 7714 | 聂翼飞 , 颜红萍 , 鹿苏微 et al. 理论指导构建Cu-O-Ti-Ov活性位点及其高效电催化还原硝酸根研究 [J]. | 催化学报 , 2024 , 59 (4) : 293-302 . |
| MLA | 聂翼飞 et al. "理论指导构建Cu-O-Ti-Ov活性位点及其高效电催化还原硝酸根研究" . | 催化学报 59 . 4 (2024) : 293-302 . |
| APA | 聂翼飞 , 颜红萍 , 鹿苏微 , 张宏伟 , 齐婷婷 , 梁诗景 et al. 理论指导构建Cu-O-Ti-Ov活性位点及其高效电催化还原硝酸根研究 . | 催化学报 , 2024 , 59 (4) , 293-302 . |
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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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