Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100466
Jiaqi Ma , Lan Li , Yiming Zhang , Jinjie Qian , Xusheng Wang
Covalent organic frameworks (COFs) are a class of stable two- or three-dimensional porous materials which are composed of ordered organic units connected by strong covalent bonds. Owing to their outstanding physical and chemical properties, COFs have garnered significant attention in recent years as promising candidates for photocatalytic reduction of CO2. In this review, we will first summarize the synthesis and structures of COFs, then provide an overview of characterization techniques used for COFs, and finally systematically review recent research progress on the photocatalytic reduction of CO2 using COFs. Fully understanding of the relations between COFs structures and photocatalytic CO2 reduction would greatly enhance the further development of this emerging area. Herein we address this gap, aiming not only to provide the latest research progress of COFs materials in the photocatalytic reduction of CO2 but also to summarize the advanced characterizations for COFs structures and illustrate how the structures guide the photocatalytic reduction of CO2 performance.
{"title":"Covalent organic frameworks: Synthesis, structures, characterizations and progress of photocatalytic reduction of CO2","authors":"Jiaqi Ma , Lan Li , Yiming Zhang , Jinjie Qian , Xusheng Wang","doi":"10.1016/j.cjsc.2024.100466","DOIUrl":"10.1016/j.cjsc.2024.100466","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs) are a class of stable two- or three-dimensional porous materials which are composed of ordered organic units connected by strong covalent bonds. Owing to their outstanding physical and chemical properties, COFs have garnered significant attention in recent years as promising candidates for photocatalytic reduction of CO<sub>2</sub>. In this review, we will first summarize the synthesis and structures of COFs, then provide an overview of characterization techniques used for COFs, and finally systematically review recent research progress on the photocatalytic reduction of CO<sub>2</sub> using COFs. Fully understanding of the relations between COFs structures and photocatalytic CO<sub>2</sub> reduction would greatly enhance the further development of this emerging area. Herein we address this gap, aiming not only to provide the latest research progress of COFs materials in the photocatalytic reduction of CO<sub>2</sub> but also to summarize the advanced characterizations for COFs structures and illustrate how the structures guide the photocatalytic reduction of CO<sub>2</sub> performance.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100466"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161884","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}
Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100458
Yihu Ke , Shuai Wang , Fei Jin , Guangbo Liu , Zhiliang Jin , Noritatsu Tsubaki
The effective separation ability of photogenerated carriers plays a crucial role in catalytic hydrogen production. Establishing a heterojunction structure is an effective means to overcome the limited carrier separation ability of some single catalysts. In this paper, Cu, graphdiyne (GDY) and NiCoMoO4 are successfully coupled to construct a composite photocatalyst NCY-15%. The addition of sheet GDY effectively prevents the aggregation of NiCoMoO4, increases the number of active sites, and enhances the light-trapping ability of the composite catalyst. The synergistic interaction of S-scheme heterojunction and Ohmic junction heterojunction between Cu, GDY and NiCoMoO4 provides a unique transfer pathway for electrons, facilitating the rapid separation of photogenerated carriers and accelerating electron transfer, while retaining electrons with strong reducing capacity to participate in hydrogen production, thereby increasing the hydrogen evolution rate. This provides a new way for the development of GDY based photocatalysts.
{"title":"Charge transfer optimization: Role of Cu-graphdiyne/NiCoMoO4 S-scheme heterojunction and Ohmic junction","authors":"Yihu Ke , Shuai Wang , Fei Jin , Guangbo Liu , Zhiliang Jin , Noritatsu Tsubaki","doi":"10.1016/j.cjsc.2024.100458","DOIUrl":"10.1016/j.cjsc.2024.100458","url":null,"abstract":"<div><div>The effective separation ability of photogenerated carriers plays a crucial role in catalytic hydrogen production. Establishing a heterojunction structure is an effective means to overcome the limited carrier separation ability of some single catalysts. In this paper, Cu, graphdiyne (GDY) and NiCoMoO<sub>4</sub> are successfully coupled to construct a composite photocatalyst NCY-15%. The addition of sheet GDY effectively prevents the aggregation of NiCoMoO<sub>4</sub>, increases the number of active sites, and enhances the light-trapping ability of the composite catalyst. The synergistic interaction of S-scheme heterojunction and Ohmic junction heterojunction between Cu, GDY and NiCoMoO<sub>4</sub> provides a unique transfer pathway for electrons, facilitating the rapid separation of photogenerated carriers and accelerating electron transfer, while retaining electrons with strong reducing capacity to participate in hydrogen production, thereby increasing the hydrogen evolution rate. This provides a new way for the development of GDY based photocatalysts.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100458"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161858","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}
Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100427
Muhammad Riaz , Rakesh Kumar Gupta , Di Sun , Mohammad Azam , Ping Cui
The development of effective adsorbent materials for capturing organic dyes and iodine is crucial to reduce the environmental impact and ensure human health. In this context, a two-dimensional (2D) Co3-based metal-organic framework SDU-CP-7 (SDU = Shandong University, CP = coordination polymer) was rationally designed with 4-(4-carboxyphenyl)-1,2,4-triazole (Hcpt) and 2,4,6-tri(4-pyridinyl)-1,3,5-triazine (tpt) as organic linkers. The SDU-CP-7 was comprehensively characterized using single-crystal X-ray diffraction analysis, thermogravimetric analysis, Fourier transform infrared spectroscopy, Raman spectroscopy, powder X-ray diffraction analysis and UV-vis spectroscopy. Molecular docking was conducted to elucidate potential binding sites on SDU-CP-7 for effective interactions with RhB and ST. Featuring negatively charged surface and trigonal microporous channels, SDU-CP-7 exhibits excellent adsorption capacities for organic dyes (919.2 mg/g for Rhodamine B and 1565 mg/g for Safranine T) as well as iodine (563.0 mg/g in solution and 1100 mg/g in the vapor phase). The exceptional adsorption performance of SDU-CP-7 for cationic dyes can be ascribed to the electrostatic interaction facilitated by negatively charged zeta potential and the size-matching principle, whereas the pyridine active sites in channels significantly enhance the binding affinity for iodine. Moreover, SDU-CP-7 can serve as chromatographic column filters for the rapid adsorption and separation of dyes. The results demonstrate excellent selective adsorption performance of SDU-CP-7, highlighting its potential for environmental and industrial applications.
开发捕捉有机染料和碘的有效吸附材料对于减少环境影响和确保人类健康至关重要。在此背景下，以 4-(4-羧基苯基)-1,2,4-三唑（Hcpt）和 2,4,6-三(4-吡啶基)-1,3,5-三嗪（tpt）为有机连接体，合理设计了一种二维（2D）Co 基金属有机框架 SDU-CP-。使用单晶 X 射线衍射分析、热重分析、傅立叶变换红外光谱、喇曼光谱、粉末 X 射线衍射分析和紫外可见光谱对 SDU-CP- 进行了全面表征。通过分子对接，阐明了 SDU-CP- 与 RhB 和 ST 有效相互作用的潜在结合位点。SDU-CP- 具有带负电荷的表面和三棱形微孔通道，对有机染料（罗丹明 B 为 919.2 毫克/克，莎呋宁 T 为 1565 毫克/克）和碘（溶液中为 563.0 毫克/克，气相中为 1100 毫克/克）具有出色的吸附能力。SDU-CP- 对阳离子染料的优异吸附性能可归因于带负电的 Zeta 电位和尺寸匹配原理所促进的静电相互作用，而通道中的吡啶活性位点则显著增强了对碘的结合亲和力。此外，SDU-CP- 还可用作色谱柱过滤器，用于快速吸附和分离染料。研究结果表明，SDU-CP- 具有出色的选择性吸附性能，在环境和工业应用方面具有巨大潜力。
{"title":"Selective adsorption of organic dyes and iodine by a two-dimensional cobalt(II) metal-organic framework","authors":"Muhammad Riaz , Rakesh Kumar Gupta , Di Sun , Mohammad Azam , Ping Cui","doi":"10.1016/j.cjsc.2024.100427","DOIUrl":"10.1016/j.cjsc.2024.100427","url":null,"abstract":"<div><div>The development of effective adsorbent materials for capturing organic dyes and iodine is crucial to reduce the environmental impact and ensure human health. In this context, a two-dimensional (2D) Co<sub>3</sub>-based metal-organic framework SDU-CP-<strong>7</strong> (SDU = Shandong University, CP = coordination polymer) was rationally designed with 4-(4-carboxyphenyl)-1,2,4-triazole (Hcpt) and 2,4,6-tri(4-pyridinyl)-1,3,5-triazine (tpt) as organic linkers. The SDU-CP-<strong>7</strong> was comprehensively characterized using single-crystal X-ray diffraction analysis, thermogravimetric analysis, Fourier transform infrared spectroscopy, Raman spectroscopy, powder X-ray diffraction analysis and UV-vis spectroscopy. Molecular docking was conducted to elucidate potential binding sites on SDU-CP-<strong>7</strong> for effective interactions with RhB and ST. Featuring negatively charged surface and trigonal microporous channels, SDU-CP-<strong>7</strong> exhibits excellent adsorption capacities for organic dyes (919.2 mg/g for Rhodamine B and 1565 mg/g for Safranine T) as well as iodine (563.0 mg/g in solution and 1100 mg/g in the vapor phase). The exceptional adsorption performance of SDU-CP-<strong>7</strong> for cationic dyes can be ascribed to the electrostatic interaction facilitated by negatively charged zeta potential and the size-matching principle, whereas the pyridine active sites in channels significantly enhance the binding affinity for iodine. Moreover, SDU-CP-<strong>7</strong> can serve as chromatographic column filters for the rapid adsorption and separation of dyes. The results demonstrate excellent selective adsorption performance of SDU-CP-<strong>7</strong>, highlighting its potential for environmental and industrial applications.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100427"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142266452","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}
Pub Date : 2024-12-01DOI: 10.1016/j.cjsc.2024.100473
Xin Wang , Changzhao Chen , Qishen Wang , Kai Dai
Graphene quantum dots (GQDs) are a novel type of carbon dot material that has significant application value in the field of catalysis due to their non-toxic, stable, abundant surface functional groups, and quantum confinement effects. A unique composite photocatalyst was constructed by modifying GQDs onto Bi2MoO6 (BMO) microsphere-shaped nano petals using simple hydrothermal and sintering techniques. The structural and morphological characterization results indicate that GQDs with the size of 10 nm are well dispersed on BMO nanosheets, forming close contacts, which can greatly improve the separation efficiency of photo-generated electron-hole pairs under visible light irradiation. In the evaluation of the catalytic performance of BPA solution (20 mg/L) with a catalyst content of 20 mg under a simulated light source with a power of 300 W, the best degradation performance was achieved by a photocatalyst (G6/BMO) with the GQDs mass ratio of 6%, which degraded over 95% of BPA under visible light within 120 min, while pure BMO only degraded about 45% of BPA during the same time period. Even if the 400 nm filter is removed and directly exposed to Xe lamp radiation, the degradation performance of the optimal composite catalyst is only slightly improved, indicating that the current GQDs/BMO composite catalyst has extremely strong visible light catalytic activity. The improvement of catalytic performance comes from the effective separation of electron-hole pairs caused by the absorption of electrons by GQDs, and the introduction of GQDs to reduce the band gap and enhance visible light absorption, both of which are beneficial for catalytic reactions. Free radical capture and electron spin resonance (ESR) tests indicate that ·OH and ·O2− are the main active species for BPA degradation. Although the current GQDs/BMO catalysts have a simple structure, their catalytic performance has significantly improved, which will guide the design of other semiconductor based photocatalysts.
{"title":"Graphene quantum dot modified Bi2MoO6 nanoflower for efficient degradation of BPA under visible light","authors":"Xin Wang , Changzhao Chen , Qishen Wang , Kai Dai","doi":"10.1016/j.cjsc.2024.100473","DOIUrl":"10.1016/j.cjsc.2024.100473","url":null,"abstract":"<div><div>Graphene quantum dots (GQDs) are a novel type of carbon dot material that has significant application value in the field of catalysis due to their non-toxic, stable, abundant surface functional groups, and quantum confinement effects. A unique composite photocatalyst was constructed by modifying GQDs onto Bi<sub>2</sub>MoO<sub>6</sub> (BMO) microsphere-shaped nano petals using simple hydrothermal and sintering techniques. The structural and morphological characterization results indicate that GQDs with the size of 10 nm are well dispersed on BMO nanosheets, forming close contacts, which can greatly improve the separation efficiency of photo-generated electron-hole pairs under visible light irradiation. In the evaluation of the catalytic performance of BPA solution (20 mg/L) with a catalyst content of 20 mg under a simulated light source with a power of 300 W, the best degradation performance was achieved by a photocatalyst (G6/BMO) with the GQDs mass ratio of 6%, which degraded over 95% of BPA under visible light within 120 min, while pure BMO only degraded about 45% of BPA during the same time period. Even if the 400 nm filter is removed and directly exposed to Xe lamp radiation, the degradation performance of the optimal composite catalyst is only slightly improved, indicating that the current GQDs/BMO composite catalyst has extremely strong visible light catalytic activity. The improvement of catalytic performance comes from the effective separation of electron-hole pairs caused by the absorption of electrons by GQDs, and the introduction of GQDs to reduce the band gap and enhance visible light absorption, both of which are beneficial for catalytic reactions. Free radical capture and electron spin resonance (ESR) tests indicate that ·OH and ·O<sub>2</sub><sup>−</sup> are the main active species for BPA degradation. Although the current GQDs/BMO catalysts have a simple structure, their catalytic performance has significantly improved, which will guide the design of other semiconductor based photocatalysts.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100473"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161882","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}
Here, we report a novel visible-light-driven I− doped Bi2O2CO3 nano-sheet photocatalyst synthesized via a facile ion exchange route at room temperature. This obtained Bi2O2CO3 nano-sheet with I− doping shows several advantages. The specific surface area of I0.875-Bi2O2CO3 is 2.16 times higher than that of Bi2O2CO3, providing more catalytic sites for the degradation reactions. Moreover, a 3.2 times photocurrent enhancement is observed in I0.875-Bi2O2CO3 compared with Bi2O2CO3, producing more photogenerated electron-hole pairs for degradation. The synergistic effect between texture property and photoelectric effect boosts the removal of organic pollutants. Under visible light illumination, I0.875-Bi2O2CO3 displays superior photocatalytic performance for the degradation of methyl orange (MO) and phenol. Notably, a phenol degradation rate, 88%, is achieved by I0.875-Bi2O2CO3 with illuminating for 60 min, which is about 29 times higher than that of pristine Bi2O2CO3. This finding may provide an opportunity to develop a promising I− doped catalyst for organic pollutants removal.
{"title":"Novel visible-light-driven I− doped Bi2O2CO3 nano-sheets fabricated via an ion exchange route for dye and phenol removal","authors":"Guanyang Zeng , Xingqiang Liu , Liangqiao Wu , Zijie Meng , Debin Zeng , Changlin Yu","doi":"10.1016/j.cjsc.2024.100462","DOIUrl":"10.1016/j.cjsc.2024.100462","url":null,"abstract":"<div><div>Here, we report a novel visible-light-driven I<sup>−</sup> doped Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> nano-sheet photocatalyst synthesized <em>via</em> a facile ion exchange route at room temperature. This obtained Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> nano-sheet with I<sup>−</sup> doping shows several advantages. The specific surface area of I<sub>0.875</sub>-Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> is 2.16 times higher than that of Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub>, providing more catalytic sites for the degradation reactions. Moreover, a 3.2 times photocurrent enhancement is observed in I<sub>0.875</sub>-Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> compared with Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub>, producing more photogenerated electron-hole pairs for degradation. The synergistic effect between texture property and photoelectric effect boosts the removal of organic pollutants. Under visible light illumination, I<sub>0.875</sub>-Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> displays superior photocatalytic performance for the degradation of methyl orange (MO) and phenol. Notably, a phenol degradation rate, 88%, is achieved by I<sub>0.875</sub>-Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> with illuminating for 60 min, which is about 29 times higher than that of pristine Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub>. This finding may provide an opportunity to develop a promising I<sup>−</sup> doped catalyst for organic pollutants removal.</div></div>","PeriodicalId":10151,"journal":{"name":"结构化学","volume":"43 12","pages":"Article 100462"},"PeriodicalIF":5.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143161856","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}
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
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, 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}
Pub Date : 2024-12-01DOI: 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 , 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}
Pub Date : 2024-12-01DOI: 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 , 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}
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
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 , 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}
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