结构化学Pub Date : 2024-12-01DOI: 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
{"title":"Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport","authors":"Jiangqi Ning, Junhan Huang, Yuhang Liu, Yanlei Chen, Qing Niu, Qingqing Lin, Yajun He, Zheyuan Liu, Yan Yu, 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}
结构化学Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100472
Linping Li , Junhui Su , Yanping Qiu , Yangqin Gao , Ning Li , Lei Ge
{"title":"Design and fabrication of ternary Au/Co3O4/ZnCdS spherical composite photocatalyst for facilitating efficient photocatalytic hydrogen production","authors":"Linping Li , Junhui Su , Yanping Qiu , Yangqin Gao , Ning Li , 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}
结构化学Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100457
Sikai Wu , Xuefei Wang , Huogen Yu
{"title":"Hydroxyl-enriched hydrous tin dioxide-coated BiVO4 with boosted photocatalytic H2O2 production","authors":"Sikai Wu , Xuefei Wang , 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}
结构化学Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100474
Xing Xiao , Yunling Jia , Wanyu Hong , Yuqing He , Yanjun Wang , Lizhi Zhao , Huiqin An , Zhen Yin
{"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 , Yunling Jia , Wanyu Hong , Yuqing He , Yanjun Wang , Lizhi Zhao , Huiqin An , 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}
结构化学Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100469
Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , Jizhou Jiang
{"title":"State-of-the-art evolution of g-C3N4-based photocatalytic applications: A critical review","authors":"Yanghanbin Zhang , Dongxiao Wen , Wei Sun , Jiahe Peng , Dezhong Yu , Xin Li , Yang Qu , 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}
结构化学Pub Date : 2024-08-29DOI: 10.1016/j.cjsc.2024.100426
Zhuoer Cai , Yinan Zhang , Xiu-Ni Hua , Baiwang Sun
{"title":"Phase transition arising from order-disorder motion in stable layered two-dimensional perovskite","authors":"Zhuoer Cai , Yinan Zhang , Xiu-Ni Hua , Baiwang Sun","doi":"10.1016/j.cjsc.2024.100426","DOIUrl":"10.1016/j.cjsc.2024.100426","url":null,"abstract":"<div><div>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 3HDMAPAPbBr<sub>4</sub> (<strong>1</strong>, 3HDMAPA is 3-(hydroxydimethylammonio)propan-1-aminium) was successfully synthesized and characterized. For <strong>1</strong>, 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.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 11","pages":"Article 100426"},"PeriodicalIF":5.9,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142177536","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}
结构化学Pub Date : 2024-08-17DOI: 10.1016/j.cjsc.2024.100411
Luyao Lu , Chen Zhu , Fei Li , Pu Wang , Xi Kang , Yong Pei , Manzhou Zhu
{"title":"Ligand effects on geometric structures and catalytic activities of atomically precise copper nanoclusters","authors":"Luyao Lu , Chen Zhu , Fei Li , Pu Wang , Xi Kang , Yong Pei , Manzhou Zhu","doi":"10.1016/j.cjsc.2024.100411","DOIUrl":"10.1016/j.cjsc.2024.100411","url":null,"abstract":"<div><p>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 Cu<sub>28</sub> nanocluster with a chemical formula of Cu<sub>28</sub>H<sub>10</sub>(SPh<sup><em>p</em></sup>OMe)<sub>18</sub>(DPPOE)<sub>3</sub>. The combination of Cu<sub>28</sub>H<sub>10</sub>(SPh<sup><em>p</em></sup>OMe)<sub>18</sub>(DPPOE)<sub>3</sub> and previously reported Cu<sub>28</sub>H<sub>10</sub>(SPh<sup><em>o</em></sup>Me)<sub>18</sub>(TPP)<sub>3</sub> 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 Cu<sub>28</sub> pair that enables the atomic-level understanding of ligand effects on the structures and properties of metal nanoclusters.</p></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 10","pages":"Article 100411"},"PeriodicalIF":5.9,"publicationDate":"2024-08-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161670","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}
结构化学Pub Date : 2024-08-16DOI: 10.1016/j.cjsc.2024.100412
Wei Chen, Pieter Cnudde
{"title":"A minireview to ketene chemistry in zeolite catalysis","authors":"Wei Chen, Pieter Cnudde","doi":"10.1016/j.cjsc.2024.100412","DOIUrl":"10.1016/j.cjsc.2024.100412","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 11","pages":"Article 100412"},"PeriodicalIF":5.9,"publicationDate":"2024-08-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142177535","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}