IF 5.9 4区化学

结构化学 Pub Date : 2024-08-14 DOI: 10.1016/j.cjsc.2024.100416

Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A.C. Carabineiro , Kangle Lv

{"title":"Effect of precursors on the structure and photocatalytic performance of g-C3N4 for NO oxidation and CO2 reduction","authors":"Liang Ma , Zhou Li , Zhiqiang Jiang , Xiaofeng Wu , Shixin Chang , Sónia A.C. Carabineiro , Kangle Lv","doi":"10.1016/j.cjsc.2024.100416","DOIUrl":"10.1016/j.cjsc.2024.100416","url":null,"abstract":"<div><div>Graphitic carbon nitride (g-C3N4, CN) is recognized as the most extensively studied organic polymeric photocatalyst for pollution control and energy conversion due to its facile synthesis and suitable electronic band structure. The aim of the present work is to explore the effect of precursors, such as urea (U, (NH2)2CO), dicyandiamide (D, C2H4N4) and melamine (M, C3H6N6), on the structure and photocatalytic activity of the obtained CN samples, denoted as UCN, DCN and MCN, respectively. The sheet-like UCN sample shows significantly enhanced photoreactivity in both NO oxidation and CO2 reduction compared to the bulk DCN and MCN materials. In addition, UCN demonstrates the ability to suppress the formation of toxic NO2 intermediate during the photocatalytic oxidation of NO. The improved photocatalytic activity of UCN can be attributed to a dual effect: first, its increased specific surface area provides more active sites for the photocatalytic reaction; second, it exhibits a stronger affinity for substrates like NO and CO2, which facilitates charge migration at the interface.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 11","pages":"Article 100416"},"PeriodicalIF":5.9,"publicationDate":"2024-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142223454","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

Nitrogen doping retrofits the coordination environment of copper single-atom catalysts for deep CO2 reduction 掺氮改造铜单原子催化剂的配位环境，实现二氧化碳深度还原

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-13 DOI: 10.1016/j.cjsc.2024.100415

Yuxiang Zhang , Jia Zhao , Sen Lin

{"title":"Nitrogen doping retrofits the coordination environment of copper single-atom catalysts for deep CO2 reduction","authors":"Yuxiang Zhang , Jia Zhao , Sen Lin","doi":"10.1016/j.cjsc.2024.100415","DOIUrl":"10.1016/j.cjsc.2024.100415","url":null,"abstract":"<div><div>The electrocatalytic CO2 reduction reaction (CO2RR) represents an effective way to address energy crises and environmental issues by converting CO2 into valuable chemicals. Single-atom catalysts (SACs) can achieve excellent catalytic activity in CO2RR. However, the study of CO2RR on SACs still poses significant challenges, especially in terms of controlling the selectivity towards the deep product such as CH4 and CH3OH. Herein, we employ density functional theory (DFT) calculations to investigate the CO2RR on Cu SAC supported on N-doped graphene (Cu-N/C) and explore the role of N dopants on the CO2RR performance. Compared to Cu SACs supported on N-doped defective graphene with double vacancy (Cu-N/C-DV), Cu SACs supported on N-doped defective graphene with single vacancy (Cu-N/C-SV) can effectively convert CO2 into the deeply reduced C1 products, including CH4 and CH3OH, thus further indicating that Cu-N/C-SV has a stronger interaction with ∗CO, which is conducive to the deep reduction of ∗CO. Increasing the coordination number of N atoms or the proximity of doping site to the Cu active site can effectively enhance the stability of catalyst and promote the adsorption of ∗CO on Cu-N/C-SV. However, this also increases the free energy of the formation of ∗CHO intermediate. The results suggest that CuC3-Nm, which contains a N atom in the second coordination shell (meta-position) of Cu SACs, has the best electrocatalytic performance of CO2RR in terms of both selectivity and catalytic activity, not only contributing to an in-depth understanding of the reaction mechanism of CO2RR on SACs but also providing insights into the design of SACs for efficient CO2RR.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 11","pages":"Article 100415"},"PeriodicalIF":5.9,"publicationDate":"2024-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142177538","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

Dynamic photoluminescence switching of carbon nitride thin films for anticounterfeiting and encryption 用于防伪和加密的氮化碳薄膜的动态光致发光开关

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-02 DOI: 10.1016/j.cjsc.2024.100410

Hang Meng , Bicheng Zhu , Ruolun Sun , Zixuan Liu , Shaowen Cao , Kan Zhang , Jiaguo Yu , Jingsan Xu

{"title":"Dynamic photoluminescence switching of carbon nitride thin films for anticounterfeiting and encryption","authors":"Hang Meng , Bicheng Zhu , Ruolun Sun , Zixuan Liu , Shaowen Cao , Kan Zhang , Jiaguo Yu , Jingsan Xu","doi":"10.1016/j.cjsc.2024.100410","DOIUrl":"10.1016/j.cjsc.2024.100410","url":null,"abstract":"<div>Photoluminescence (PL) has been increasingly applied in anticounterfeiting and encryption as counterfeiting becomes more prevalent. However, common luminescent encryption techniques are based on static PL measurements and are easy to counterfeit. In this work, we have developed a thermal vapor deposition (TVD) approach using melem as the unique starting material to synthesize highly homogeneous carbon nitride (CN) thin films featuring unique dynamic PL switching properties. After being irradiated by a white LED, the blue PL intensity of the CN film increases significantly and then fades in darkness, demonstrating excellent recyclability. Experimental results prove that CN films contain cyano groups in the structure, and density functional theory (DFT) calculations indicate that the integration of cyano groups results in traps within the bandgap of CN, suggesting that the dynamic PL switching effect is essentially associated with the fullness of the trap states. We have therefore developed an advanced luminescent device for the secure transmission of encrypted information through controlled illumination. It can be easily read with a portable UV (365 nm) lamp and effectively erased using the white LED, thereby preventing information leakage and showing great potential for many applications.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 10","pages":"Article 100410"},"PeriodicalIF":5.9,"publicationDate":"2024-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0254586124002733/pdfft?md5=1f137ee929ade0567085104ce2dada7b&pid=1-s2.0-S0254586124002733-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mesoporous CuCe dual-metal catalysts for efficient electrochemical reduction of CO2 to methane 用于将二氧化碳高效电化学还原为甲烷的介孔铜铈双金属催化剂

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100350

引用次数: 0

Deciphering the structural evolution and real active ingredients of iron oxides in photocatalytic CO2 hydrogenation 解密光催化二氧化碳加氢过程中氧化铁的结构演变和真正活性成分

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100348

{"title":"Deciphering the structural evolution and real active ingredients of iron oxides in photocatalytic CO2 hydrogenation","authors":"","doi":"10.1016/j.cjsc.2024.100348","DOIUrl":"10.1016/j.cjsc.2024.100348","url":null,"abstract":"<div>Photocatalytic CO2 hydrogenation reactions can produce high-value-added chemicals for industry, solving the environmental problems caused by excessive CO2 emissions. Iron oxides are commonly used in photocatalytic reactions due to their various structures and suitable band gaps. Nevertheless, the structural evolution and real active components during photocatalytic CO2 hydrogenation reaction are rarely studied. Herein, a variety of iron oxides including α-Fe2O3, γ-Fe2O3, Fe3O4 and FeO were derived from Prussian blue precursors to investigate the CO2 hydrogenation performance, structural evolution and active components. Especially, the typical α- and γ-Fe2O3 are converted to Fe3O4 during the reaction, while Fe/FexOy remains structurally stable. Meanwhile, it is confirmed that Fe3O4 is the main active component for CO production and the formation of hydrocarbons (CH4 and C2–C4) are highly dependent on the Fe/FexOy heterojunctions. The optimal yields of CO, CH4 and C2–C4 hydrocarbons over the best catalyst (FeFe-550) can achieve 4 mmol g−1 h−1, 350 μmol g−1 h−1 and 150 μmol g−1 h−1, respectively due to their suitable metal/oxide component distribution. This work examines the structural evolution of different iron oxide catalysts in the photocatalytic CO2 hydrogenation reaction, identifies the active components as well as reveals the relationship between components and the products, and offers valuable insights into the efficient utilization of CO2.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 8","pages":"Article 100348"},"PeriodicalIF":5.9,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141143924","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

Ni-based electrocatalysts for urea-assisted water splitting 用于脲辅助水分离的镍基电催化剂

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100373

引用次数: 0

Modulating pollutant adsorption and peroxymonosulfate activation sites on Co3O4@N,O doped-carbon shell for boosting catalytic degradation activity 调节掺杂碳壳 Co3O4@N,O 上的污染物吸附和过一硫酸盐活化位点以提高催化降解活性

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100332

{"title":"Modulating pollutant adsorption and peroxymonosulfate activation sites on Co3O4@N,O doped-carbon shell for boosting catalytic degradation activity","authors":"","doi":"10.1016/j.cjsc.2024.100332","DOIUrl":"10.1016/j.cjsc.2024.100332","url":null,"abstract":"<div>The construction of double active sites for pollutant adsorption and peroxymonosulfate (PMS) activation on the surface of catalyst is conducive to further enhancing the pollutant-removing effect. Herein, a N,O co-doped carbon-encapsulated tricobalt tetraoxide (Co3O4@N,O–C) with double active sites is prepared by a one-step laser carbonization method. The optimized Co3O4@N,O–C shows excellent tetracycline (TC) removal ability, in which the k value reaches 0.608 min−1. On the surface of Co3O4@N,O–C, TC is adsorbed to the N site, and PMS is activated at the O site. Building double active sites on the catalyst surface not only avoids competition for the active site, but also confines the pollutant molecules to the surface of the catalyst, thus shortening the migration distance between reactive oxygen species (ROS) and the pollutant and boosting the removal efficiency of pollutants. In addition, the Co3O4@N,O–C/PMS system exhibits both good resistance to environmental interference and cyclic stability. Finally, a practical continuous flow reactor based on Co3O4@N,O–C catalyst is built, which shows a stable and efficient TC degradation performance.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 8","pages":"Article 100332"},"PeriodicalIF":5.9,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141033209","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

All in one doubly pillared MXene membrane for excellent oil/water separation, pollutant removal, and anti-fouling performance 一体化双层 MXene 膜可实现出色的油水分离、污染物去除和防污性能

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100355

{"title":"All in one doubly pillared MXene membrane for excellent oil/water separation, pollutant removal, and anti-fouling performance","authors":"","doi":"10.1016/j.cjsc.2024.100355","DOIUrl":"10.1016/j.cjsc.2024.100355","url":null,"abstract":"<div>Given the diversity and complexity of coexisting oil/dyes/heavy metal ions/microorganisms in wastewater and volatile organic compounds (VOCs) in the air, developing separation materials featured in higher separation efficiency and lower energy consumption for oil and water separation, pollutant removal, and anti-fouling is urgently needed, but it remains a major challenge till now. Herein, a multifunctional Ti3C2 MXene membrane with unique double pillar support was proposed by liquid phase ultrasonication and vacuum filtration to overcome the above challenge. Introducing cetyl-trimethyl ammonium bromide (CTAB) and calcium chloride/sodium alginate (CaCl2/SA) to the MXene membrane as crossed double pillars and superhydrophilic surface increases the tolerance and wettability of the membrane. The fabricated doubly pillared MXene (d-Ti3C2) membrane exhibits superior oil/water (O/W) separation efficiency (99.76%) with flux (1.284 L m−2 h−1) for canola oil and organic dye removing efficiency for methyl blue (MB) 99.85%, malachite green (MG) 100%, and methyl violet (MV) 99.72%, respectively, which is 1.05, 1.44, 1.22, and 1.28 fold compared with pre-pillared Ti3C2 (p-Ti3C2). The superior anti-oil/dye/fouling is attributed to lower oil conglutination, high hydrophily, and antibacterial activity. The versatile MXene membrane also shows distinguished separation of VOCs (η > 99%) from polluted air. The experimental and molecular dynamics (MD) computational simulation results illustrate that the superior separation efficiency of the Ti3C2 MXene membrane is ascribed to the unique doubly pillared space channel. This study paves a new road to further research on one step integration strategy for complex O/W separation, wastewater and VOCs removal, and anti-fouling via tuning nano/macro architecture.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 8","pages":"Article 100355"},"PeriodicalIF":5.9,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141191267","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

Insight into stable, concentrated radicals from sulfur-functionalized alkyne-rich crystalline frameworks and application in solar-to-vapor conversion 深入了解硫功能化富炔烃晶体框架产生的稳定、浓缩自由基及其在太阳能-蒸汽转换中的应用

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100380

{"title":"Insight into stable, concentrated radicals from sulfur-functionalized alkyne-rich crystalline frameworks and application in solar-to-vapor conversion","authors":"","doi":"10.1016/j.cjsc.2024.100380","DOIUrl":"10.1016/j.cjsc.2024.100380","url":null,"abstract":"<div>Organic radicals feature versatile unpaired electrons key for photoelectronic and biomedical applications but remain difficult to access in stable concentrated forms. We disclose easy generation of stable, concentrated radicals from various alkynyl phenyl motifs, including 1) sulfur-functionalized alkyne-rich organic linkers in crystalline frameworks; 2) the powders of these molecules alone; 3) simple diethynylbenzenes. For Zr-based framework, the generation of radical-rich crystalline framework was achieved by thermal annealing in the range of 300–450 °C. For terminal alkynes, electron paramagnetic resonance signals (EPR, indicative of free radicals) arise after air exposure or mild heating (e.g., 70 °C). Further heating (e.g., 150 °C for 3 h) raises the radical concentrations up to 3.30 mol kg−1. For more stable internal alkynes, transformations into porous radical solids can also be triggered, albeit at higher temperatures (e.g., 250–500 °C). The resulted radical-containing solids are porous, stable to air as well as heat (up to 300–450 °C) and exhibit photothermal conversion and solar-driven water evaporation capacity. The formation of radicals can be ascribed to extensive alkyne cyclizations, forming defects, dangling bonds and the associated radicals stabilized by polycyclic π-systems.</div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 8","pages":"Article 100380"},"PeriodicalIF":5.9,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141512243","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

Reconstruction mechanism of Cu surface in CO2 reduction process 二氧化碳还原过程中铜表面的重构机制

IF 5.9 4区化学

结构化学 Pub Date : 2024-08-01 DOI: 10.1016/j.cjsc.2024.100328

引用次数: 0

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