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学者姓名：梁诗景
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Abstract ：
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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Various exposed facets can cause a huge difference in the catalytic activity. Here we prepared Co3O4 hexagonal nanosheets with exposed {112}, {112}&{111}, and {111} facets for the electrochemical nitrate reduction reactions (NO3RR). The reaction pathways of the NO3RR on Co3O4 {111} and {112} facets are clarified through in situ electrochemical characterizations and theoretical analysis. As the dominating facet of Co3O4 transforms from {112} to {111}, the rate-determining step changes from *NO2 -> *NO2H to *NO3H -> *NO2, with the energy barrier decreasing to 0.48 eV. And the {111} facet promotes the hydrogenation of NOx and NHx intermediates. Notably, the Co3O4-{111} catalyst shows exceptional NO3RR performance, achieving an NH3 yield of 5.73 mg mg(cat.)(-1) h(-1), surpassing the majority of the reported activities.
Keyword ：
ammonia synthesis ammonia synthesis cobalt tetroxide cobalt tetroxide electrochemical nitratereduction electrochemical nitratereduction facet effect facet effect facet transformation engineering facet transformation engineering
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| GB/T 7714 | Lu, Suwei , Lin, Guanting , Yan, Hongping et al. In Situ Facet Transformation Engineering over Co3O4 for Highly Efficient Electroreduction of Nitrate to Ammonia [J]. | ACS CATALYSIS , 2024 , 14 (19) : 14887-14894 . |
| MLA | Lu, Suwei et al. "In Situ Facet Transformation Engineering over Co3O4 for Highly Efficient Electroreduction of Nitrate to Ammonia" . | ACS CATALYSIS 14 . 19 (2024) : 14887-14894 . |
| APA | Lu, Suwei , Lin, Guanting , Yan, Hongping , Li, Yuhang , Qi, Tingting , Li, Yuanjin et al. In Situ Facet Transformation Engineering over Co3O4 for Highly Efficient Electroreduction of Nitrate to Ammonia . | ACS CATALYSIS , 2024 , 14 (19) , 14887-14894 . |
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Electrocatalytic nitrate reduction reaction (NO3RR) has been capturing immense interest in the industrial application of ammonia synthesis, and it involves complex reaction routes accompanied by multi-electron transfer, thus causing a challenge to achieve high efficiency for catalysts. Herein, we customized the Cu-O-Ti-Ov (oxygen vacancy) structure on the Cu/TiO2 catalyst, identified through density functional theory (DFT) calculations as the synergic active site for NO3RR. It is found that Cu-O-Ti-Ov site facilitates the adsorption/association of NOx- and promotes the hydrogenation of NO3- to NH3 via adsorbed *H species. This effectively suppresses the competing hydrogen evolution reaction (HER) and exhibits a lower reaction energy barrier for NO3RR, with the reaction pathways: NO3* -> NO2* -> HONO* -> NO* -> *NOH -> *N -> *NH -> *NH2 -> *NH3 -> NH3. The optimized Cu/TiO2 catalyst with rich Cu-O-Ti-Ov sites achieves an NH3 yield rate of 3046.5 mu g h-1 mgcat-1 at -1.0 V vs. RHE, outperforming most of the reported activities. Furthermore, the construction of Cu-O-Ti-Ov sites significantly mitigates the leaching of Cu species, enhancing the stability of the Cu/TiO2 catalyst. Additionally, a mechanistic study, using in situ characterizations and various comparative experiments, further confirms the strong synergy between Cu, Ti, and Ov sites, which is consistent with previous DFT calculations. This study provides a new strategy for designing efficient and stable electrocatalysts in the field of ammonia synthesis. Published by Elsevier B.V. All rights reserved.
Keyword ：
Ammonia synthesis Ammonia synthesis Cu-O-Ti-O v site Cu-O-Ti-O v site Cu/TiO 2 catalyst Cu/TiO 2 catalyst Electrocatalytic nitrate reduction Electrocatalytic nitrate reduction Synergic catalytic effect Synergic catalytic effect
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| GB/T 7714 | Nie, Yifei , Yan, Hongping , Lu, Suwei et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction [J]. | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 : 293-302 . |
| MLA | Nie, Yifei et al. "Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction" . | CHINESE JOURNAL OF CATALYSIS 59 (2024) : 293-302 . |
| APA | Nie, Yifei , Yan, Hongping , Lu, Suwei , Zhang, Hongwei , Qi, Tingting , Liang, Shijing et al. Theory-guided construction of Cu-O-Ti-Ov active sites on Cu/TiO2 catalysts for efficient electrocatalytic nitrate reduction . | CHINESE JOURNAL OF CATALYSIS , 2024 , 59 , 293-302 . |
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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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Electrocatalytic nitrogen (N2) 2 ) reduction to ammonia (NH3) 3 ) reaction (eNRR) supplies a promising alternative to the Haber-Bosch technology. However, the dissociation of N---N - -- N bond hinders its development. Herein, sulfur vacancies are introduced into FeS2 2 for promoting N2 2 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 2 2 pi* orbital, thus facilitating the cracking of inert N2 2 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 2 surface follows the distal and alternating hybrid pathway. Also, the water molecules in the electrolyte facilitate the first hydrogenation of N2 2 (*N2 2 -> *NNH). Notably, FeS2 2 with rich sulfur vacancies exhibits an excellent NH3 3 yield rate of 67.5 mu g h- 1 mg cat.-1 , which outperforms most of the reported eNRR activities of Fe-based catalysts.
Keyword ：
Density functional theory Density functional theory Electrocatalytic nitrogen reduction Electrocatalytic nitrogen reduction N 2 activation N 2 activation Sulfur defect Sulfur defect
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| GB/T 7714 | Lin, Jiawei , Lin, Xiaoyun , Lu, Suwei et al. Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia [J]. | CHEMICAL ENGINEERING SCIENCE , 2024 , 300 . |
| MLA | Lin, Jiawei et al. "Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia" . | CHEMICAL ENGINEERING SCIENCE 300 (2024) . |
| APA | Lin, Jiawei , Lin, Xiaoyun , Lu, Suwei , Liao, Wanru , Qi, Tingting , Liang, Shijing et al. Sulfur defect engineering boosted nitrogen activation over FeS2 for efficient electrosynthesis of ammonia . | CHEMICAL ENGINEERING SCIENCE , 2024 , 300 . |
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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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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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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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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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