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Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100453
Jiangqi Ning, Junhan Huang, Yuhang Liu, Yanlei Chen, Qing Niu, Qingqing Lin, Yajun He, Zheyuan Liu, Yan Yu, Liuyi Li
Targeted electron transfer to catalytically active site for CO2 reduction is promising for enhancing the efficiency of artificial photosynthesis. Here, we demonstrate a design of an alkyl-linked heterostructure composing of TiO2 and a Cu-porphyrin-based covalent organic framework (TiO2@CuPorTT-COF) for the photoreduction of CO2 with H2O. Through specific coordination effect, the alkyl chain bridges TiO2 and Cu moiety in COF. Upon light illumination, the photoinduced electrons in TiO2 can be directionally transported across the interface along the alkyl chain to the Cu active sites to reduce adsorbed CO2, while the left holes are consumed by the H2O oxidation, enhancing the spatial separation and utilization of electron-hole pairs. Accordingly, the TiO2@CuPorTT-COF enables remarkably superior catalytic activities over the counterpart without the alkyl bridge for electron transfer with 5 times of CO production rate. An apparent quantum efficiency of 0.455% at 380 nm is achieved. Moreover, a dynamic evolution of Cu active site for CO2 reduction is revealed, which can be promoted by the targeting electron transport approach. This work provides a targeted electron transport strategy for constructing photocatalysts.
{"title":"Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport","authors":"Jiangqi Ning,&nbsp;Junhan Huang,&nbsp;Yuhang Liu,&nbsp;Yanlei Chen,&nbsp;Qing Niu,&nbsp;Qingqing Lin,&nbsp;Yajun He,&nbsp;Zheyuan Liu,&nbsp;Yan Yu,&nbsp;Liuyi Li","doi":"10.1016/j.cjsc.2024.100453","DOIUrl":"10.1016/j.cjsc.2024.100453","url":null,"abstract":"<div><div>Targeted electron transfer to catalytically active site for CO<sub>2</sub> reduction is promising for enhancing the efficiency of artificial photosynthesis. Here, we demonstrate a design of an alkyl-linked heterostructure composing of TiO<sub>2</sub> and a Cu-porphyrin-based covalent organic framework (TiO<sub>2</sub>@CuPorTT-COF) for the photoreduction of CO<sub>2</sub> with H<sub>2</sub>O. Through specific coordination effect, the alkyl chain bridges TiO<sub>2</sub> and Cu moiety in COF. Upon light illumination, the photoinduced electrons in TiO<sub>2</sub> can be directionally transported across the interface along the alkyl chain to the Cu active sites to reduce adsorbed CO<sub>2</sub>, while the left holes are consumed by the H<sub>2</sub>O oxidation, enhancing the spatial separation and utilization of electron-hole pairs. Accordingly, the TiO<sub>2</sub>@CuPorTT-COF enables remarkably superior catalytic activities over the counterpart without the alkyl bridge for electron transfer with 5 times of CO production rate. An apparent quantum efficiency of 0.455% at 380 nm is achieved. Moreover, a dynamic evolution of Cu active site for CO<sub>2</sub> reduction is revealed, which can be promoted by the targeting electron transport approach. This work provides a targeted electron transport strategy for constructing photocatalysts.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100453"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacial channel design on the charge migration for photoelectrochemical applications 关于 PEC 应用中电荷迁移的界面通道设计
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100398
Shengdong Sun, Cheng Wang, Shikuo Li
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引用次数: 0
Design and fabrication of ternary Au/Co3O4/ZnCdS spherical composite photocatalyst for facilitating efficient photocatalytic hydrogen production
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100472
Linping Li , Junhui Su , Yanping Qiu , Yangqin Gao , Ning Li , Lei Ge
Promoting efficient carrier separation and transfer can largely enhance photocatalytic performance and inhibit photo-corrosion. In this work, ZnCdS (ZCS) microspheres were obtained by a self-assembly strategy, and the Au/Co3O4/ZCS composites were synthesized by a modified photo-deposition method (loading Co3O4 and Au onto the surface of ZnCdS). The synergistic effect between the S-scheme heterojunction (Co3O4/ZCS) and Schottky junction (Au/ZCS) can effectively promote the generation and separation of photoelectrons and holes, thus enhancing the photocatalytic activity. Under visible light, the efficient photocatalysts showed hydrogen production activities up to 2525 μmol g−1 h−1, which is 2.24 times higher than that of Co3O4/ZCS and 6.92 times higher than that of pure ZnCdS. DFT calculations indicate that the built-in electric field between Co3O4/ZCS provides the driving force for efficient electron-hole separation, and the Au nanoparticles (NPs) act as electron collectors at the interface of ZnCdS to capture the electrons, which effectively prolongs the lifetime of photoelectrons and further enhances the photocatalytic hydrogen production activity.
{"title":"Design and fabrication of ternary Au/Co3O4/ZnCdS spherical composite photocatalyst for facilitating efficient photocatalytic hydrogen production","authors":"Linping Li ,&nbsp;Junhui Su ,&nbsp;Yanping Qiu ,&nbsp;Yangqin Gao ,&nbsp;Ning Li ,&nbsp;Lei Ge","doi":"10.1016/j.cjsc.2024.100472","DOIUrl":"10.1016/j.cjsc.2024.100472","url":null,"abstract":"<div><div>Promoting efficient carrier separation and transfer can largely enhance photocatalytic performance and inhibit photo-corrosion. In this work, ZnCdS (ZCS) microspheres were obtained by a self-assembly strategy, and the Au/Co<sub>3</sub>O<sub>4</sub>/ZCS composites were synthesized by a modified photo-deposition method (loading Co<sub>3</sub>O<sub>4</sub> and Au onto the surface of ZnCdS). The synergistic effect between the S-scheme heterojunction (Co<sub>3</sub>O<sub>4</sub>/ZCS) and Schottky junction (Au/ZCS) can effectively promote the generation and separation of photoelectrons and holes, thus enhancing the photocatalytic activity. Under visible light, the efficient photocatalysts showed hydrogen production activities up to 2525 μmol g<sup>−1</sup> h<sup>−1</sup>, which is 2.24 times higher than that of Co<sub>3</sub>O<sub>4</sub>/ZCS and 6.92 times higher than that of pure ZnCdS. DFT calculations indicate that the built-in electric field between Co<sub>3</sub>O<sub>4</sub>/ZCS provides the driving force for efficient electron-hole separation, and the Au nanoparticles (NPs) act as electron collectors at the interface of ZnCdS to capture the electrons, which effectively prolongs the lifetime of photoelectrons and further enhances the photocatalytic hydrogen production activity.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100472"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161880","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Hydroxyl-enriched hydrous tin dioxide-coated BiVO4 with boosted photocatalytic H2O2 production
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100457
Sikai Wu , Xuefei Wang , Huogen Yu
The rapid decomposition of H2O2 on the surface of inorganic photocatalyst (BiVO4) and insufficient proton supply from water leads to a low photosynthetic yield of H2O2. Herein, hydrous tin dioxide (HSnO) with massive hydroxyl groups is coated on the BiVO4 surface to greatly improve the photocatalytic H2O2 activity via simultaneous realization of providing sufficient protons and inhibiting H2O2 decomposition. After coating HSnO, Au nanoparticles as the O2-reduction active sites are selectively deposited on the (010) facet of BiVO4 to synthesize Au/BiVO4@HSnO photocatalyst. The resulting Au/BiVO4@HSnO photocatalyst exhibits excellent H2O2-production performance, in which the photogenerated H2O2 concentration (210.7 μmol L−1) is about 4.8 times higher than that of Au/BiVO4 after 2 h light irradiation in pure water. The outstanding photocatalytic performance can be attributed to simultaneous enhancement of H2O2 generation and the suppression of H2O2 decomposition by HSnO coating. Specifically, the HSnO coating with massive hydroxyl groups provides enough protons to promote the catalytic transformation of O2 into H2O2 on Au nanoparticles. More importantly, this coating not only allows water molecules to effectively permeate onto BiVO4 surface for rapid oxidation reaction, but also greatly inhibits the reverse reaction of H2O2 decomposition via decreasing its affinity with BiVO4 surface. This research offers new insights for boosting photocatalytic H2O2 production through surface coating strategy.
{"title":"Hydroxyl-enriched hydrous tin dioxide-coated BiVO4 with boosted photocatalytic H2O2 production","authors":"Sikai Wu ,&nbsp;Xuefei Wang ,&nbsp;Huogen Yu","doi":"10.1016/j.cjsc.2024.100457","DOIUrl":"10.1016/j.cjsc.2024.100457","url":null,"abstract":"<div><div>The rapid decomposition of H<sub>2</sub>O<sub>2</sub> on the surface of inorganic photocatalyst (BiVO<sub>4</sub>) and insufficient proton supply from water leads to a low photosynthetic yield of H<sub>2</sub>O<sub>2</sub>. Herein, hydrous tin dioxide (HSnO) with massive hydroxyl groups is coated on the BiVO<sub>4</sub> surface to greatly improve the photocatalytic H<sub>2</sub>O<sub>2</sub> activity via simultaneous realization of providing sufficient protons and inhibiting H<sub>2</sub>O<sub>2</sub> decomposition. After coating HSnO, Au nanoparticles as the O<sub>2</sub>-reduction active sites are selectively deposited on the (010) facet of BiVO<sub>4</sub> to synthesize Au/BiVO<sub>4</sub>@HSnO photocatalyst. The resulting Au/BiVO<sub>4</sub>@HSnO photocatalyst exhibits excellent H<sub>2</sub>O<sub>2</sub>-production performance, in which the photogenerated H<sub>2</sub>O<sub>2</sub> concentration (210.7 μmol L<sup>−1</sup>) is about 4.8 times higher than that of Au/BiVO<sub>4</sub> after 2 h light irradiation in pure water. The outstanding photocatalytic performance can be attributed to simultaneous enhancement of H<sub>2</sub>O<sub>2</sub> generation and the suppression of H<sub>2</sub>O<sub>2</sub> decomposition by HSnO coating. Specifically, the HSnO coating with massive hydroxyl groups provides enough protons to promote the catalytic transformation of O<sub>2</sub> into H<sub>2</sub>O<sub>2</sub> on Au nanoparticles. More importantly, this coating not only allows water molecules to effectively permeate onto BiVO<sub>4</sub> surface for rapid oxidation reaction, but also greatly inhibits the reverse reaction of H<sub>2</sub>O<sub>2</sub> decomposition via decreasing its affinity with BiVO<sub>4</sub> surface. This research offers new insights for boosting photocatalytic H<sub>2</sub>O<sub>2</sub> production through surface coating strategy.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100457"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161857","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sulfur-defective ZnIn2S4 nanosheets decorated by TiO2 nanosheets with exposed {001} facets to accelerate charge transfer for efficient photocatalytic hydrogen evolution
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100474
Xing Xiao , Yunling Jia , Wanyu Hong , Yuqing He , Yanjun Wang , Lizhi Zhao , Huiqin An , Zhen Yin
Efficient separation and transfer of photogenerated carriers is one of the important factors for improving photocatalytic H2 production from water splitting. In this work, ZnIn2S4 nanosheets (NSs) with sulfur defect (Vs-ZIS) and TiO2 NSs with exposed {001} facets (001-TiO2 NSs) are fabricated firstly, then the novel 001-TiO2/Vs-ZIS heterojunction is constructed by employing NH4HCO3 as a binder, in which NH4+ attracts the 001-TiO2 and Vs-ZIS NSs to contact with each other and forms a compact 2D/2D heterostructure. Benefit from the suitable band structure of Vs-ZIS and 001-TiO2, the photoinduced electrons on 001-TiO2 recombine with the photoinduced holes on Vs-ZIS following Z-scheme mechanism, leading to the remarkable separation of photogenerated carriers. In addition, the synergistic effects of unique 2D/2D structure, highly active {001} facets and sulfur defect also contribute to the efficient separation of photogenerated carriers and enhanced photocatalytic activity in 001-TiO2/Vs-ZIS system. The obtained 2D/2D 001-TiO2/Vs-ZIS photocatalyst exhibits an outstanding H2 evolution rate of 17113 μmol g−1 h−1, which is approximately 1426- and 3-fold compared to those of 001-TiO2 NSs and Vs-ZIS NSs, respectively.
{"title":"Sulfur-defective ZnIn2S4 nanosheets decorated by TiO2 nanosheets with exposed {001} facets to accelerate charge transfer for efficient photocatalytic hydrogen evolution","authors":"Xing Xiao ,&nbsp;Yunling Jia ,&nbsp;Wanyu Hong ,&nbsp;Yuqing He ,&nbsp;Yanjun Wang ,&nbsp;Lizhi Zhao ,&nbsp;Huiqin An ,&nbsp;Zhen Yin","doi":"10.1016/j.cjsc.2024.100474","DOIUrl":"10.1016/j.cjsc.2024.100474","url":null,"abstract":"<div><div>Efficient separation and transfer of photogenerated carriers is one of the important factors for improving photocatalytic H<sub>2</sub> production from water splitting. In this work, ZnIn<sub>2</sub>S<sub>4</sub> nanosheets (NSs) with sulfur defect (Vs-ZIS) and TiO<sub>2</sub> NSs with exposed {001} facets (001-TiO<sub>2</sub> NSs) are fabricated firstly, then the novel 001-TiO<sub>2</sub>/Vs-ZIS heterojunction is constructed by employing NH<sub>4</sub>HCO<sub>3</sub> as a binder, in which NH<sub>4</sub><sup>+</sup> attracts the 001-TiO<sub>2</sub> and Vs-ZIS NSs to contact with each other and forms a compact 2D/2D heterostructure. Benefit from the suitable band structure of Vs-ZIS and 001-TiO<sub>2</sub>, the photoinduced electrons on 001-TiO<sub>2</sub> recombine with the photoinduced holes on Vs-ZIS following Z-scheme mechanism, leading to the remarkable separation of photogenerated carriers. In addition, the synergistic effects of unique 2D/2D structure, highly active {001} facets and sulfur defect also contribute to the efficient separation of photogenerated carriers and enhanced photocatalytic activity in 001-TiO<sub>2</sub>/Vs-ZIS system. The obtained 2D/2D 001-TiO<sub>2</sub>/Vs-ZIS photocatalyst exhibits an outstanding H<sub>2</sub> evolution rate of 17113 μmol g<sup>−1</sup> h<sup>−1</sup>, which is approximately 1426- and 3-fold compared to those of 001-TiO<sub>2</sub> NSs and Vs-ZIS NSs, respectively.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100474"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161883","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-12-01 DOI: 10.1016/j.cjsc.2024.100469
Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , Jizhou Jiang
g-C3N4 is a promising non-metallic photocatalyst recognized for its unique structural and physicochemical properties. Recent reviews have addressed g-C3N4-based photocatalysis; however, the rapid progress in big data and artificial intelligence has significantly accelerated the design, synthesis, and optimization of these materials. Machine learning, theoretical simulations, and advanced in-situ characterization techniques have deepened our understanding of their photocatalytic mechanisms. This review critically evaluates advancements in g-C3N4-based photocatalysts over the last two to three years, focusing on strategies to improve photogenerated charge separation, expand light absorption, and enhance stability and catalytic efficiency. It discusses cutting-edge in-situ characterization methods alongside machine learning approaches for predicting and optimizing applications in photocatalytic H2 evolution, CO2 reduction, pollutant degradation, H2O2 production, and nitrogen fixation. Finally, it proposes prospective strategies for further enhancing the performance of g-C3N4-based photocatalysts, aiming to guide the design of high-performance two-dimensional carbon-based photocatalysts.
{"title":"State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review","authors":"Yanghanbin Zhang ,&nbsp;Dongxiao Wen ,&nbsp;Wei Sun ,&nbsp;Jiahe Peng ,&nbsp;Dezhong Yu ,&nbsp;Xin Li ,&nbsp;Yang Qu ,&nbsp;Jizhou Jiang","doi":"10.1016/j.cjsc.2024.100469","DOIUrl":"10.1016/j.cjsc.2024.100469","url":null,"abstract":"<div><div>g-C<sub>3</sub>N<sub>4</sub> is a promising non-metallic photocatalyst recognized for its unique structural and physicochemical properties. Recent reviews have addressed g-C<sub>3</sub>N<sub>4</sub>-based photocatalysis; however, the rapid progress in big data and artificial intelligence has significantly accelerated the design, synthesis, and optimization of these materials. Machine learning, theoretical simulations, and advanced <em>in-situ</em> characterization techniques have deepened our understanding of their photocatalytic mechanisms. This review critically evaluates advancements in g-C<sub>3</sub>N<sub>4</sub>-based photocatalysts over the last two to three years, focusing on strategies to improve photogenerated charge separation, expand light absorption, and enhance stability and catalytic efficiency. It discusses cutting-edge <em>in-situ</em> characterization methods alongside machine learning approaches for predicting and optimizing applications in photocatalytic H<sub>2</sub> evolution, CO<sub>2</sub> reduction, pollutant degradation, H<sub>2</sub>O<sub>2</sub> production, and nitrogen fixation. Finally, it proposes prospective strategies for further enhancing the performance of g-C<sub>3</sub>N<sub>4</sub>-based photocatalysts, aiming to guide the design of high-performance two-dimensional carbon-based photocatalysts.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100469"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161881","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Phase transition arising from order-disorder motion in stable layered two-dimensional perovskite 稳定的层状二维过氧化物中的有序-无序运动引起的相变
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-29 DOI: 10.1016/j.cjsc.2024.100426
Zhuoer Cai , Yinan Zhang , Xiu-Ni Hua , Baiwang Sun
In recent years, organic-inorganic hybrid materials are widely designed and synthesized as switching materials for temperature response. However, due to the change of molecular arrangement inside the crystal during solid-solid phase transition, the distortion of crystal lattice and the great change of lattice parameters are often caused, which result in a poor repeatability and short life. Thus, designing phase change materials with small lattice changes helps to improve product life. In this article, a novel organic-inorganic hybrid material 3HDMAPAPbBr4 (1, 3HDMAPA is 3-(hydroxydimethylammonio)propan-1-aminium) was successfully synthesized and characterized. For 1, organic cations filled in the van der Waals gap are connected by hydrogen bonds with halogens in the two-dimensional inorganic layer, forming a stable sandwich structure. During the solid-solid phase transition driven by temperature, the changes of inorganic skeleton are relatively small, and the disorder movement of organic cations does not affect the existence of hydrogen bonds, maintaining a relatively stable crystal structure. In addition, electrical property, optical property and crystal structures are analyzed and discussed in detail. We believe that our work will contribute to the development and application of phase change materials in response materials.
近年来,有机-无机杂化材料作为温度响应开关材料被广泛设计和合成。然而,在固-固相变过程中,由于晶体内部分子排列的变化,往往会引起晶格的畸变和晶格参数的巨大变化,从而导致重复性差、寿命短。因此,设计晶格变化小的相变材料有助于提高产品寿命。本文成功合成并表征了一种新型有机无机杂化材料 3HDMAPAPbBr(3HDMAPA 是 3-(羟基二甲基氨基)丙-1-氨基)。其中,范德华间隙中填充的有机阳离子通过氢键与二维无机层中的卤素连接,形成稳定的夹层结构。在温度驱动的固-固相变过程中,无机骨架的变化相对较小,有机阳离子的无序运动不影响氢键的存在,保持了相对稳定的晶体结构。此外,还对电学性质、光学性质和晶体结构进行了详细分析和讨论。我们相信,我们的工作将有助于相变材料在响应材料中的开发和应用。
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引用次数: 0
Ligand effects on geometric structures and catalytic activities of atomically precise copper nanoclusters 配体对原子精度纳米铜簇几何结构和催化活性的影响
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-17 DOI: 10.1016/j.cjsc.2024.100411
Luyao Lu , Chen Zhu , Fei Li , Pu Wang , Xi Kang , Yong Pei , Manzhou Zhu

The ligand effects have been extensively investigated in Au and Ag nanoclusters, while corresponding research efforts focusing on Cu nanoclusters remain relatively insufficient. Such a scarcity could primarily be attributed to the inherent instability of Cu nanoclusters relative to their Au/Ag analogues. In this work, we report the controllable preparation and structural determination of a hydride-containing Cu28 nanocluster with a chemical formula of Cu28H10(SPhpOMe)18(DPPOE)3. The combination of Cu28H10(SPhpOMe)18(DPPOE)3 and previously reported Cu28H10(SPhoMe)18(TPP)3 constructs a structure-correlated cluster pair with comparable structures and properties. Accordingly, the ligand effects in directing the geometric structures and physicochemical properties (including optical absorptions and catalytic activities towards the selected hydrogenation) of copper nanoclusters were analyzed. Overall, this work presents a structure-correlated Cu28 pair that enables the atomic-level understanding of ligand effects on the structures and properties of metal nanoclusters.

配体效应已在金纳米团簇和银纳米团簇中得到了广泛研究,而针对铜纳米团簇的相应研究仍相对不足。造成这种不足的主要原因是,相对于金/银类似物,铜纳米团簇具有固有的不稳定性。在这项工作中,我们报告了含氢化物的 Cu28 纳米簇的可控制备和结构测定,其化学式为 Cu28H10(SPhpOMe)18(DPPOE)3。 Cu28H10(SPhpOMe)18(DPPOE)3 与之前报告的 Cu28H10(SPhoMe)18(TPP)3 的组合构建了结构相关的簇对,具有相似的结构和性质。因此,该研究分析了配体对纳米铜簇几何结构和理化性质(包括光学吸收和对所选氢化反应的催化活性)的影响。总之,这项研究提出了一对结构相关的 Cu28,有助于在原子水平上理解配体对金属纳米簇结构和性质的影响。
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引用次数: 0
A minireview to ketene chemistry in zeolite catalysis 沸石催化中的烯酮化学小览
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-16 DOI: 10.1016/j.cjsc.2024.100412
Wei Chen, Pieter Cnudde
Ketene and its derivatives, including surface acetate and acylium ion, are pivotal intermediates in zeolite catalysis, facilitating the conversion of C1 molecules into various chemicals. Understanding the formation, transformation, and function of ketene in zeolite catalysis is fundamental for comprehending and enhancing numerous chemical processes. Recent research advances have contributed significantly to a deeper molecular-level comprehension of how ketene affects the catalytic efficacy of zeolites, thereby playing a crucial role in the advancement of more efficient and selective catalytic processes. This minireview aims to provide an overview of ketene chemistry in zeolite catalysis, delineate the reaction network involving ketene, elucidate the role of ketene in zeolite-catalyzed reactions, and summarize the methods for characterizing ketene in zeolite environments.
烯酮及其衍生物(包括表面醋酸盐和酰基离子)是沸石催化过程中的关键中间体,可促进 C1 分子转化为各种化学物质。了解沸石催化过程中酮的形成、转化和功能对于理解和改进众多化学过程至关重要。最近的研究进展极大地促进了对烯酮如何影响沸石催化效能的分子层面的深入理解,从而在推进更高效、更具选择性的催化过程中发挥了至关重要的作用。这篇微型综述旨在概述沸石催化中的烯酮化学,描述涉及烯酮的反应网络,阐明烯酮在沸石催化反应中的作用,并总结沸石环境中烯酮的表征方法。
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引用次数: 0
Shining bright: Revolutionary near-unity NIR phosphorescent metal nanoclusters 闪耀光芒革命性的近统一近红外磷光金属纳米团簇
IF 5.9 4区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Pub Date : 2024-08-14 DOI: 10.1016/j.cjsc.2024.100417
Rakesh Kumar Gupta, Zhi Wang, Di Sun
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引用次数: 0
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