Pub Date : 2024-12-01Epub Date: 2024-07-25DOI: 10.1016/j.jcis.2024.07.192
Yating Cui, Siyu Ji, Yujie Zhu, Jingyu Xi
The practical applications of lithium sulfur batteries (LSBs) are hindered by notorious shuttle effect and sluggish conversion kinetics of intermediate polysulfides. Herein, Mo2C-Co heterogeneous particles decorated two-dimensional (2D) carbon nanosheets grown on hollow carbon microtubes (CCC@MCC) are synthesized. Three-dimensional (3D) carbon framework with Mo2C-Co heterogeneous particles combines the conductivity, adsorption and catalysis, effectively trapping and accelerating the conversion of polysulfides. As evidenced experimentally, the hetero-structured Mo2C-Co with high Li+ diffusion coefficient enables uniform precipitation and complete oxidation of Li2S. Meanwhile, CCC@MCC is found to have multiple application possibilities for lithium-sulfur batteries. As an interlayer, the cells deliver an excellent capacity of 881.1 mAh/g at 2C and still retain 438.2 mAh/g after 500 cycles under the low temperature of 0 ℃. As a sulfur carrier, the cell with a sulfur loading of 7.0 mg cm-2 exhibits a high area capacity of 5.3 mAh cm-2. This work provides an effective strategy to prepare heterostructured material and imaginatively exploit the application potential of it.
{"title":"Mo<sub>2</sub>C-Co heterostructure with carbon nanosheets decorated carbon microtubules: Different means for high-performance lithium-sulfur batteries.","authors":"Yating Cui, Siyu Ji, Yujie Zhu, Jingyu Xi","doi":"10.1016/j.jcis.2024.07.192","DOIUrl":"10.1016/j.jcis.2024.07.192","url":null,"abstract":"<p><p>The practical applications of lithium sulfur batteries (LSBs) are hindered by notorious shuttle effect and sluggish conversion kinetics of intermediate polysulfides. Herein, Mo<sub>2</sub>C-Co heterogeneous particles decorated two-dimensional (2D) carbon nanosheets grown on hollow carbon microtubes (CCC@MCC) are synthesized. Three-dimensional (3D) carbon framework with Mo<sub>2</sub>C-Co heterogeneous particles combines the conductivity, adsorption and catalysis, effectively trapping and accelerating the conversion of polysulfides. As evidenced experimentally, the hetero-structured Mo<sub>2</sub>C-Co with high Li<sup>+</sup> diffusion coefficient enables uniform precipitation and complete oxidation of Li<sub>2</sub>S. Meanwhile, CCC@MCC is found to have multiple application possibilities for lithium-sulfur batteries. As an interlayer, the cells deliver an excellent capacity of 881.1 mAh/g at 2C and still retain 438.2 mAh/g after 500 cycles under the low temperature of 0 ℃. As a sulfur carrier, the cell with a sulfur loading of 7.0 mg cm<sup>-2</sup> exhibits a high area capacity of 5.3 mAh cm<sup>-2</sup>. This work provides an effective strategy to prepare heterostructured material and imaginatively exploit the application potential of it.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141791573","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
It is critical and challenging to develop highly active and low cost bifunctional electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) in water electrolysis. Herein, we propose cerium-vanadium-based hollow nanopillar arrays supported on nickel foam (CeV-HNA/NF) as bifunctional HER/OER electrocatalysts, which are prepared by etching the V metal-organic framework with Ce salt and then pyrolyzing. Etching results in multidimensional optimizations of electrocatalysts, covering substantial oxygen vacancies, optimized electronic configurations, and an open-type structure of hollow nanopillar arrays, which contribute to accelerating the charge transfer rate, regulating the adsorption energy of H/O-containing reaction intermediates, and fully exposing the active sites. The reconstruction of the electrocatalyst is also accelerated by Ce doping, which results in highly active hydroxy vanadium oxide interfaces. Therefore, extremely low overpotentials of 170 and 240 mV under a current density of 100 mA cm-2 are achieved for the HER and OER under alkaline conditions, respectively, with long-term stability for 300 h. An electrolysis cell with CeV-HNA/NF as both the cathode and anode delivers a small voltage of 1.53 V to achieve water electrolysis under 10 mA cm-2, accompanied by superior durability for 150 h. This design provides an innovative way to develop advanced bifunctional electrocatalysts for overall water electrolysis.
为电解水中的氢/氧进化反应(HER/OER)开发高活性、低成本的双功能电催化剂既重要又具有挑战性。在此,我们提出以铈钒为基础、以泡沫镍为支撑的中空纳米柱阵列(CeV-HNA/NF)作为双功能 HER/OER 电催化剂,其制备方法是用铈盐蚀刻 V 金属有机框架,然后进行热解。蚀刻工艺可对电催化剂进行多维优化,包括大量的氧空位、优化的电子构型以及中空纳米柱阵列的开放型结构,这些都有助于加快电荷转移速率、调节含 H/O 反应中间产物的吸附能以及充分暴露活性位点。掺杂 Ce 还能加速电催化剂的重构,从而形成高活性的羟基氧化钒界面。因此,在 100 mA cm-2 的电流密度下,碱性条件下的 HER 和 OER 可分别达到 170 mV 和 240 mV 的极低过电位,并可长期稳定运行 300 小时;同时使用 CeV-HNA/NF 作为阴极和阳极的电解池可在 10 mA cm-2 的电流密度下提供 1.53 V 的小电压实现水电解,并可在 150 小时内保持卓越的耐久性。
{"title":"Multiple-perspective design of hollow-structured cerium-vanadium-based nanopillar arrays for enhanced overall water electrolysis.","authors":"Yan Qin, Caizheng Wang, Xinran Hou, Huijie Zhang, Zhaoyang Tan, Xiaobin Wang, Jingde Li, Feichao Wu","doi":"10.1016/j.jcis.2024.07.104","DOIUrl":"10.1016/j.jcis.2024.07.104","url":null,"abstract":"<p><p>It is critical and challenging to develop highly active and low cost bifunctional electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) in water electrolysis. Herein, we propose cerium-vanadium-based hollow nanopillar arrays supported on nickel foam (CeV-HNA/NF) as bifunctional HER/OER electrocatalysts, which are prepared by etching the V metal-organic framework with Ce salt and then pyrolyzing. Etching results in multidimensional optimizations of electrocatalysts, covering substantial oxygen vacancies, optimized electronic configurations, and an open-type structure of hollow nanopillar arrays, which contribute to accelerating the charge transfer rate, regulating the adsorption energy of H/O-containing reaction intermediates, and fully exposing the active sites. The reconstruction of the electrocatalyst is also accelerated by Ce doping, which results in highly active hydroxy vanadium oxide interfaces. Therefore, extremely low overpotentials of 170 and 240 mV under a current density of 100 mA cm<sup>-2</sup> are achieved for the HER and OER under alkaline conditions, respectively, with long-term stability for 300 h. An electrolysis cell with CeV-HNA/NF as both the cathode and anode delivers a small voltage of 1.53 V to achieve water electrolysis under 10 mA cm<sup>-2</sup>, accompanied by superior durability for 150 h. This design provides an innovative way to develop advanced bifunctional electrocatalysts for overall water electrolysis.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141632255","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-06DOI: 10.1016/j.jcis.2024.09.024
The water pollution caused by the abuse of antibiotics has significant harmful effects on the environment and human health. The photo-Fenton process is currently the most effective method for removing antibiotics from water, but it encounters challenges such as inadequate response to visible light, low yield and utilization of photogenerated electrons, and slow electron transport. In this study, spin state regulation was introduced into the photo-Fenton process, and the spin state of Co3+ was regulated through Ce displacement doping. The intermediate-spin state Ce-LaCoO3 could degrade 91.6 % of tetracycline within 120 min in the photo-Fenton system, which is 15.2 % higher than that of low-spin state LaCoO3. The improved degradation effect is attributed to the reasons that Ce-LaCoO3 in the intermediate-spin state have lower band gap, better charge transfer ability, and stronger adsorption capacity of H2O2, which can accelerate the redox cycle of Co2+/Co3+ and promote the generation of ·OH. This study presents a unique strategy for synthesizing efficient photo-Fenton materials to treat antibiotic wastewater effectively.
{"title":"Optimizing 3d electronic structure of LaCoO3 based on spin state tuning for enhancing photo-Fenton activity on tetracycline degradation","authors":"","doi":"10.1016/j.jcis.2024.09.024","DOIUrl":"10.1016/j.jcis.2024.09.024","url":null,"abstract":"<div><p>The water pollution caused by the abuse of antibiotics has significant harmful effects on the environment and human health. The photo-Fenton process is currently the most effective method for removing antibiotics from water, but it encounters challenges such as inadequate response to visible light, low yield and utilization of photogenerated electrons, and slow electron transport. In this study, spin state regulation was introduced into the photo-Fenton process, and the spin state of Co<sup>3+</sup> was regulated through Ce displacement doping. The intermediate-spin state Ce-LaCoO<sub>3</sub> could degrade 91.6 % of tetracycline within 120 min in the photo-Fenton system, which is 15.2 % higher than that of low-spin state LaCoO<sub>3</sub>. The improved degradation effect is attributed to the reasons that Ce-LaCoO<sub>3</sub> in the intermediate-spin state have lower band gap, better charge transfer ability, and stronger adsorption capacity of H<sub>2</sub>O<sub>2</sub>, which can accelerate the redox cycle of Co<sup>2+</sup>/Co<sup>3+</sup> and promote the generation of ·OH. This study presents a unique strategy for synthesizing efficient photo-Fenton materials to treat antibiotic wastewater effectively.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142151137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-05DOI: 10.1016/j.jcis.2024.09.030
The human perception and learning heavily rely on the visual system, where the retina plays a vital role in preprocessing visual information. Developing neuromorphic vision hardware is based on imitating the neurobiological functions of the retina. In this work, an optoelectronic neuron is developed by combining a gate-modulated PDVT-10 channel with a volatile threshold switching memristor, enabling the achievement of optoelectronic performance through a resistance-matching mechanism. The optoelectronic spiking neuron exhibits the ability to alter its spiking behavior in a manner resembling that of a retina. Incorporating electrical and optical modulation, the artificial neuron accurately replicates neuronal signal transmission in a biologically manner. Moreover, it demonstrates inhibition of neuronal firing during darkness and activation upon exposure to light. Finally, the evaluation of a perceptron spiking neural network utilizing these leaky integrate-and-fire neurons is conducted through simulation to assess its capability in classifying image recognition algorithms. This research offers a hopeful direction for the development of easily expandable and hierarchically structured spiking electronics, broadening the range of potential applications in biomimetic vision within the emerging field of neuromorphic hardware.
{"title":"Optoelectronic neuron based on transistor combined with volatile threshold switching memristors for neuromorphic computing","authors":"","doi":"10.1016/j.jcis.2024.09.030","DOIUrl":"10.1016/j.jcis.2024.09.030","url":null,"abstract":"<div><p>The human perception and learning heavily rely on the visual system, where the retina plays a vital role in preprocessing visual information. Developing neuromorphic vision hardware is based on imitating the neurobiological functions of the retina. In this work, an optoelectronic neuron is developed by combining a gate-modulated PDVT-10 channel with a volatile threshold switching memristor, enabling the achievement of optoelectronic performance through a resistance-matching mechanism. The optoelectronic spiking neuron exhibits the ability to alter its spiking behavior in a manner resembling that of a retina. Incorporating electrical and optical modulation, the artificial neuron accurately replicates neuronal signal transmission in a biologically manner. Moreover, it demonstrates inhibition of neuronal firing during darkness and activation upon exposure to light. Finally, the evaluation of a perceptron spiking neural network utilizing these leaky integrate-and-fire neurons is conducted through simulation to assess its capability in classifying image recognition algorithms. This research offers a hopeful direction for the development of easily expandable and hierarchically structured spiking electronics, broadening the range of potential applications in biomimetic vision within the emerging field of neuromorphic hardware.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142151138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-05DOI: 10.1016/j.jcis.2024.09.034
Expanding the application field of polyolefin materials through functionalization has been a research hotspot in the past three decades. Here, a TiO2-supported anilinenaphthoquinone nickel catalyst was assembled and applied for in situ ethylene polymerization with high activity (>2000 kg mol–1h−1) to produce ultra-high molecular weight polyethylene (UHMWPE)/TiO2 composites with unique physicochemical performance. The UHMWPE/TiO2 composite films and fibers prepared by in-situ ethylene polymerization are superior to the samples from the blend system in issues such as TiO2 dispersibility, mechanical property, and photocatalytic degradability. The mechanical properties (strength up to 26.8 cN/dtex, modulus up to 1248.8 cN/dtex) of the obtained UHMWPE/TiO2 composite fibers are significantly improved with a very low dosage of TiO2 (as low as 1.4 wt‰). Moreover, UHMWPE/TiO2 composites obtained by coating Al2O3 and SiO2 on the surface of TiO2 not only retain the strong absorption of ultraviolet rays, but also effectively weaken the photocatalytic degradation effect.
{"title":"Nickel-catalyzed in situ synthesis of UHMWPE/TiO2 composites with enhanced mechanical properties and adjustable photocatalytic degradabilities","authors":"","doi":"10.1016/j.jcis.2024.09.034","DOIUrl":"10.1016/j.jcis.2024.09.034","url":null,"abstract":"<div><p>Expanding the application field of polyolefin materials through functionalization has been a research hotspot in the past three decades. Here, a TiO<sub>2</sub>-supported anilinenaphthoquinone nickel catalyst was assembled and applied for in situ ethylene polymerization with high activity (>2000 kg mol<sup>–1</sup>h<sup>−1</sup>) to produce ultra-high molecular weight polyethylene (UHMWPE)/TiO<sub>2</sub> composites with unique physicochemical performance. The UHMWPE/TiO<sub>2</sub> composite films and fibers prepared by in-situ ethylene polymerization are superior to the samples from the blend system in issues such as TiO<sub>2</sub> dispersibility, mechanical property, and photocatalytic degradability. The mechanical properties (strength up to 26.8 cN/dtex, modulus up to 1248.8 cN/dtex) of the obtained UHMWPE/TiO<sub>2</sub> composite fibers are significantly improved with a very low dosage of TiO<sub>2</sub> (as low as 1.4 wt‰). Moreover, UHMWPE/TiO<sub>2</sub> composites obtained by coating Al<sub>2</sub>O<sub>3</sub> and SiO<sub>2</sub> on the surface of TiO<sub>2</sub> not only retain the strong absorption of ultraviolet rays, but also effectively weaken the photocatalytic degradation effect.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142150636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-05DOI: 10.1016/j.jcis.2024.09.009
Silicon (Si) is considered as one of the most potential commercial materials for the next-generation lithium-ion batteries (LIBs) owing to its high theoretical capacity and low voltage platform. However, the severe volume expansion and poor electric conductivity of Si anodes limit the practical application. Herein, a hierarchical porous hard carbon@Si@soft carbon (PHC@Si@SC) material was prepared by a chemical vapor deposition (CVD) and following calcination process. The differences in capacities and initial Coulombic efficiencies (ICEs) resulting from variations in silane deposition are demonstrated using PHC@Si as a model. To improve the cycling performance, a cheap pitch-derived soft carbon was introduced to protect the nano-Si to suppress the volume expansion. The formed PHC@Si@SC anode delivers a high capacity of 1625 mAh g−1 and a high ICE of 86.8%, attributed to the excellent cooperation of hard and soft carbon. The capacity retention is 55% after 100 cycles with a harsh N/P ratio of 1.1 in a PHC@Si@SC||NCM811 full cell. This work provides a strategy, which is easy to scale up for practical application.
{"title":"A hierarchical porous hard carbon@Si@soft carbon material for advanced lithium-ion batteries","authors":"","doi":"10.1016/j.jcis.2024.09.009","DOIUrl":"10.1016/j.jcis.2024.09.009","url":null,"abstract":"<div><p>Silicon (Si) is considered as one of the most potential commercial materials for the next-generation lithium-ion batteries (LIBs) owing to its high theoretical capacity and low voltage platform. However, the severe volume expansion and poor electric conductivity of Si anodes limit the practical application. Herein, a hierarchical porous hard carbon@Si@soft carbon (PHC@Si@SC) material was prepared by a chemical vapor deposition (CVD) and following calcination process. The differences in capacities and initial Coulombic efficiencies (ICEs) resulting from variations in silane deposition are demonstrated using PHC@Si as a model. To improve the cycling performance, a cheap pitch-derived soft carbon was introduced to protect the nano-Si to suppress the volume expansion. The formed PHC@Si@SC anode delivers a high capacity of 1625 mAh g<sup>−1</sup> and a high ICE of 86.8%, attributed to the excellent cooperation of hard and soft carbon. The capacity retention is 55% after 100 cycles with a harsh N/P ratio of 1.1 in a PHC@Si@SC||NCM811 full cell. This work provides a strategy, which is easy to scale up for practical application.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142151040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-03DOI: 10.1016/j.jcis.2024.09.012
Photocatalytic water splitting technology for H2 production represents a promising and sustainable approach to clean energy generation. In this study, a high concentration of oxygen vacancies was introduced into tungsten trioxide (WO3) to create a vacancy-rich layer. This modified WO3 (WO3-x) was then combined with N-doped Zn0.6Cd0.4S through a hydrothermal synthesis, resulting in the formation of a Z-scheme heterojunction composite aimed at enhancing photocatalytic performance. Under visible light, the H2 production activity of the composite reached an impressive 8.52 mmol·g−1 without adding co-catalyst Pt. This corresponds to enhancements of 7.82 and 4.39 times the production yield of pure ZCS and ZCSN, respectively. However, the hydrogen production increased to 21.98 mmol·g−1 when Pt was added as a co-catalyst. Furthermore, an array of characterizations were employed to elucidate the presence of oxygen vacancies and the establishment of the Z-scheme heterojunction. This structural enhancement significantly facilitates the utilization of photo-generated electrons while effectively preventing photo-corrosion of ZCSN, thus improving material stability. Our study provides a new scheme for the incorporation of oxygen-rich vacancy and the construction of Z-scheme heterojunction, demonstrating a synergistic effect that greatly advances photocatalytic performance.
用于生产 H2 的光催化水分离技术是一种前景广阔的可持续清洁能源生产方法。在这项研究中,在三氧化钨(WO3)中引入了高浓度的氧空位,以形成富空位层。然后,通过水热合成法将这种改性 WO3(WO3-x)与掺杂 N 的 Zn0.6Cd0.4S 结合在一起,形成了一种 Z 型异质结复合材料,旨在提高光催化性能。在不添加助催化剂铂的情况下,该复合材料在可见光下的产氢活性达到了惊人的 8.52 mmol-g-1。然而,当加入铂作为助催化剂时,氢气产量增加到 21.98 mmol-g-1。此外,还采用了一系列表征方法来阐明氧空位的存在和 Z 型异质结的建立。这种结构的增强极大地促进了光生电子的利用,同时有效地防止了 ZCSN 的光腐蚀,从而提高了材料的稳定性。我们的研究为富氧空位的掺入和 Z 型异质结的构建提供了一种新的方案,展示了一种协同效应,大大提高了光催化性能。
{"title":"In-situ construction of N-doped Zn0.6Cd0.4S/oxygen vacancy-rich WO3 Z-scheme heterojunction compound for boosting photocatalytic hydrogen production","authors":"","doi":"10.1016/j.jcis.2024.09.012","DOIUrl":"10.1016/j.jcis.2024.09.012","url":null,"abstract":"<div><p>Photocatalytic water splitting technology for H<sub>2</sub> production represents a promising and sustainable approach to clean energy generation. In this study, a high concentration of oxygen vacancies was introduced into tungsten trioxide (WO<sub>3</sub>) to create a vacancy-rich layer. This modified WO<sub>3</sub> (WO<sub>3-x</sub>) was then combined with <em>N</em>-doped Zn<sub>0.6</sub>Cd<sub>0.4</sub>S through a hydrothermal synthesis, resulting in the formation of a Z-scheme heterojunction composite aimed at enhancing photocatalytic performance. Under visible light, the H<sub>2</sub> production activity of the composite reached an impressive 8.52 mmol·g<sup>−1</sup> without adding co-catalyst Pt. This corresponds to enhancements of 7.82 and 4.39 times the production yield of pure ZCS and ZCSN, respectively. However, the hydrogen production increased to 21.98 mmol·g<sup>−1</sup> when Pt was added as a co-catalyst. Furthermore, an array of characterizations were employed to elucidate the presence of oxygen vacancies and the establishment of the Z-scheme heterojunction. This structural enhancement significantly facilitates the utilization of photo-generated electrons while effectively preventing photo-corrosion of ZCSN, thus improving material stability. Our study provides a new scheme for the incorporation of oxygen-rich vacancy and the construction of Z-scheme heterojunction, demonstrating a synergistic effect that greatly advances photocatalytic performance.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142144756","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-03DOI: 10.1016/j.jcis.2024.09.019
Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca1/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca1/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.
由于单原子固体基催化剂(SASBC)具有高活性并能最大限度地利用碱性位点,因此其制备受到了广泛关注。目前,已报道的 SASBC 制备方法,如两步还原策略和升华捕获策略,都需要较高的温度。如此高的活化温度容易造成碱金属或碱土金属原子的升华损失,并对支撑结构造成破坏。本文制备了一种新型 SASBC--Ca1/UiO-67-BPY,在室温下将碱土金属 Ca 位点固定在富 N 金属有机框架 UiO-67-BPY 上。结果表明,Ca 单原子的原子构型在框架中由两个 N 原子配位。所获得的 Ca SASBC 具有有序结构,在苯甲醛和丙二腈的 Knoevenagel 反应中表现出 87.2% 的高产率。此外,由于 Ca 单原子位点锚定在 UiO-67-BPY 上,Ca1/UiO-67-BPY 催化剂在循环过程中也表现出良好的稳定性。这项工作可能会为设计用于不同碱催化反应的 SASBC 提供新的见解。
{"title":"Calcium single atoms stabilized by nitrogen coordination in metal–organic frameworks as efficient solid base catalysts","authors":"","doi":"10.1016/j.jcis.2024.09.019","DOIUrl":"10.1016/j.jcis.2024.09.019","url":null,"abstract":"<div><p>Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca<sub>1</sub>/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal–organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca<sub>1</sub>/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142144769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-03DOI: 10.1016/j.jcis.2024.09.006
Enabling highly-efficient multiplex-optimization photocatalysts is critical to overcome the bottlenecks of hydrogen evolution reaction efficiency and photostability. Herein, novel CoS/Sv-ZnIn2S4/MoS2 composites are successfully synthesized through an in situ technique. Taking advantage of the synergistic effect of sulfur vacancy, Schottky-type MoS2/Sv-ZnIn2S4 junction and Ohmic-type CoS/Sv-ZnIn2S4 junction, the light absorption, electron/hole separation efficiency, charge transfer rate and hydrogen reduction reaction dynamic can be significantly enhanced. As a result, an impressive photocatalytic hydrogen evolution rate of 18.43 mmol g−1 h−1 is achieved under the visible-light irradiation. Furthermore, apparent quantum efficiencies of 72.14 % and 9.91 % are also achieved under 350 and 420 nm monochromatic light irradiation. This work presents an in situ perspective to design multiplex-optimization photocatalytic system for highly-efficient hydrogen production.
{"title":"Synergistically-mediated highly-efficient visible-light-driven hydrogen evolution activity using Ohmic/Schottky-type dual-junctions and sulfur vacancy","authors":"","doi":"10.1016/j.jcis.2024.09.006","DOIUrl":"10.1016/j.jcis.2024.09.006","url":null,"abstract":"<div><p>Enabling highly-efficient multiplex-optimization photocatalysts is critical to overcome the bottlenecks of hydrogen evolution reaction efficiency and photostability. Herein, novel CoS/S<sub>v</sub>-ZnIn<sub>2</sub>S<sub>4</sub>/MoS<sub>2</sub> composites are successfully synthesized through an <em>in situ</em> technique. Taking advantage of the synergistic effect of sulfur vacancy, Schottky-type MoS<sub>2</sub>/S<sub>v</sub>-ZnIn<sub>2</sub>S<sub>4</sub> junction and Ohmic-type CoS/S<sub>v</sub>-ZnIn<sub>2</sub>S<sub>4</sub> junction, the light absorption, electron/hole separation efficiency, charge transfer rate and hydrogen reduction reaction dynamic can be significantly enhanced. As a result, an impressive photocatalytic hydrogen evolution rate of 18.43 mmol g<sup>−1</sup> h<sup>−1</sup> is achieved under the visible-light irradiation. Furthermore, apparent quantum efficiencies of 72.14 % and 9.91 % are also achieved under 350 and 420 nm monochromatic light irradiation. This work presents an <em>in situ</em> perspective to design multiplex-optimization photocatalytic system for highly-efficient hydrogen production.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142151039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-09-03DOI: 10.1016/j.jcis.2024.09.003
The photocatalytic hydrogen production performance of semiconductor materials can be improved by co-catalyst modification. In most of the studies, the size of the co-catalyst is relatively small compared to the primary catalyst. However, in this study, we employed a novel strategy by synthesizing a relatively large-sized Cu2MoS4 as the co-catalyst and in situ loading smaller-sized Zn0.5Cd0.5S onto Cu2MoS4, verifying that Cu2MoS4 enhances the photocatalytic hydrogen production efficiency of Zn0.5Cd0.5S. It can be observed by scanning electron microscopy (SEM) that the lateral size of 2D Cu2MoS4 is at least 50 times larger than the Zn0.5Cd0.5S nanoparticle particle size. In addition, Density Functional Theory (DFT) calculations have demonstrated that the active site for hydrogen production in the composite is located in Cu2MoS4. The large-sized of Cu2MoS4 not only provides more active sites but also broadens the electron transport channel, which is conducive to promoting the transfer of photogenerated electrons from Zn0.5Cd0.5S. This work enriches the study of large-sized materials as co-catalyst and provides a strategy for the construction of composite catalysts.
{"title":"A special coupling strategy: Cu2MoS4 as a large-sized co-catalyst for promoting photocatalytic hydrogen production performance","authors":"","doi":"10.1016/j.jcis.2024.09.003","DOIUrl":"10.1016/j.jcis.2024.09.003","url":null,"abstract":"<div><p>The photocatalytic hydrogen production performance of semiconductor materials can be improved by co-catalyst modification. In most of the studies, the size of the co-catalyst is relatively small compared to the primary catalyst. However, in this study, we employed a novel strategy by synthesizing a relatively large-sized Cu<sub>2</sub>MoS<sub>4</sub> as the co-catalyst and in situ loading smaller-sized Zn<sub>0.5</sub>Cd<sub>0.5</sub>S onto Cu<sub>2</sub>MoS<sub>4</sub>, verifying that Cu<sub>2</sub>MoS<sub>4</sub> enhances the photocatalytic hydrogen production efficiency of Zn<sub>0.5</sub>Cd<sub>0.5</sub>S. It can be observed by scanning electron microscopy (SEM) that the lateral size of 2D Cu<sub>2</sub>MoS<sub>4</sub> is at least 50 times larger than the Zn<sub>0.5</sub>Cd<sub>0.5</sub>S nanoparticle particle size. In addition, Density Functional Theory (DFT) calculations have demonstrated that the active site for hydrogen production in the composite is located in Cu<sub>2</sub>MoS<sub>4</sub>. The large-sized of Cu<sub>2</sub>MoS<sub>4</sub> not only provides more active sites but also broadens the electron transport channel, which is conducive to promoting the transfer of photogenerated electrons from Zn<sub>0.5</sub>Cd<sub>0.5</sub>S. This work enriches the study of large-sized materials as co-catalyst and provides a strategy for the construction of composite catalysts.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142144757","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}