Journal of Colloid and Interface Science最新文献

The critical effect of different additive interlayer anions on NiFe-LDH for direct seawater splitting: A theoretical study 不同添加剂层间阴离子对 NiFe-LDH 直接拆分海水的临界效应：理论研究。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-15 DOI: 10.1016/j.jcis.2024.11.069

Lu Wang , Ying Wang , Liang Zhou , Jing-yao Liu , Zhijian Wu

Direct seawater electrolysis greatly alleviates the shortage of freshwater resources, emerging as a promising approach for hydrogen production. Unfortunately, the slow kinetics of oxygen evolution reaction (OER) and the complex seawater environment, especially the chloride oxidation reaction (ClOR), pose significant challenges for the design of direct seawater electrolysis catalysts. For the sake of enhancing corrosion resistance to chloride ions (Cl⁻), an alkaline environment is settled for increasing the potential difference between OER and competitive ClOR. NiFe-LDH has been recognized as a benchmark catalyst in alkaline environment owing to its unique advantages. However, in strongly alkaline environment, the deposition of Mg(OH)₂ and Ca(OH)₂ at the cathode limits the overall efficiency of direct seawater electrolysis. In this study, we have investigated the underlying effect of four different interlayer anions (PO₄³⁻, SO₄²⁻, CO₃²⁻, and NO₃⁻) on the OER activity, selectivity, and pH application range of NiFe-LDH using density functional theory. Furthermore, we have explored the intrinsic correlations between electronic structure and catalytic performance. Our results confirm that the interlayer anions play a favorable role in promoting OER activity. Among them, NiFe-LDH with PO₄³⁻ remarkably outperforms the other interlayer anions in terms of OER activity and selectivity, reducing the OER overpotential (η) to 0.29 V and overcoming the limitations associated with high pH conditions. Most importantly, there is a linear relationship between η and the charge transferred from the interlayer anion to the catalyst surface (ΔQ_tot), implying that the interlayer anions are able to regulate the catalytic activity through essential charge transfer. This study provides theoretical insights into the design and development of advanced OER catalysts that can simultaneously suppress ClOR for direct seawater electrolysis.

直接海水电解大大缓解了淡水资源短缺的问题，是一种前景广阔的制氢方法。遗憾的是，由于氧进化反应（OER）动力学缓慢，海水环境复杂，尤其是氯离子氧化反应（ClOR），给直接海水电解催化剂的设计带来了巨大挑战。为了增强对氯离子（Cl-）的耐腐蚀性，需要在碱性环境中提高 OER 与竞争性 ClOR 之间的电位差。NiFe-LDH 因其独特的优势已被公认为碱性环境中的基准催化剂。然而，在强碱性环境中，阴极的 Mg(OH)2 和 Ca(OH)2 沉积限制了直接电解海水的整体效率。在本研究中，我们利用密度泛函理论研究了四种不同的层间阴离子（PO43-、SO42-、CO32- 和 NO3-）对 NiFe-LDH 的 OER 活性、选择性和 pH 应用范围的潜在影响。此外，我们还探索了电子结构与催化性能之间的内在联系。我们的研究结果证实，层间阴离子在促进 OER 活性方面起着有利的作用。其中，含有 PO43- 的 NiFe-LDH 在 OER 活性和选择性方面明显优于其他层间阴离子，能将 OER 过电位 (η) 降低到 0.29 V，并克服了高 pH 条件下的限制。最重要的是，η 与从层间阴离子转移到催化剂表面的电荷（ΔQtot）之间存在线性关系，这意味着层间阴离子能够通过基本的电荷转移来调节催化活性。这项研究为设计和开发可同时抑制直接电解海水中 ClOR 的先进 OER 催化剂提供了理论依据。

{"title":"The critical effect of different additive interlayer anions on NiFe-LDH for direct seawater splitting: A theoretical study","authors":"Lu Wang , Ying Wang , Liang Zhou , Jing-yao Liu , Zhijian Wu","doi":"10.1016/j.jcis.2024.11.069","DOIUrl":"10.1016/j.jcis.2024.11.069","url":null,"abstract":"<div><div>Direct seawater electrolysis greatly alleviates the shortage of freshwater resources, emerging as a promising approach for hydrogen production. Unfortunately, the slow kinetics of oxygen evolution reaction (OER) and the complex seawater environment, especially the chloride oxidation reaction (ClOR), pose significant challenges for the design of direct seawater electrolysis catalysts. For the sake of enhancing corrosion resistance to chloride ions (Cl−), an alkaline environment is settled for increasing the potential difference between OER and competitive ClOR. NiFe-LDH has been recognized as a benchmark catalyst in alkaline environment owing to its unique advantages. However, in strongly alkaline environment, the deposition of Mg(OH)2 and Ca(OH)2 at the cathode limits the overall efficiency of direct seawater electrolysis. In this study, we have investigated the underlying effect of four different interlayer anions (PO43−, SO42−, CO32−, and NO3−) on the OER activity, selectivity, and pH application range of NiFe-LDH using density functional theory. Furthermore, we have explored the intrinsic correlations between electronic structure and catalytic performance. Our results confirm that the interlayer anions play a favorable role in promoting OER activity. Among them, NiFe-LDH with PO43− remarkably outperforms the other interlayer anions in terms of OER activity and selectivity, reducing the OER overpotential (η) to 0.29 V and overcoming the limitations associated with high pH conditions. Most importantly, there is a linear relationship between η and the charge transferred from the interlayer anion to the catalyst surface (ΔQtot), implying that the interlayer anions are able to regulate the catalytic activity through essential charge transfer. This study provides theoretical insights into the design and development of advanced OER catalysts that can simultaneously suppress ClOR for direct seawater electrolysis.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 43-52"},"PeriodicalIF":9.4,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646242","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}

引用次数: 0

Efficient urea electrosynthesis from nitrite and CO2 reduction on single W atom catalyst 在单 W 原子催化剂上利用亚硝酸盐和二氧化碳还原进行高效尿素电合成。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-15 DOI: 10.1016/j.jcis.2024.11.075

Di Yuan , Yafu Jiang , Wenyu Du , Dongwei Ma , Ke Chu

Electroreduction of CO₂ and NO₂⁻ to urea (ECNU) provides a fascinating method for concurrently migrating polluted NO₂⁻ and producing value-added urea. In this study, atomically dispersed W on MoS₂ (W₁/MoS₂) is designed as an efficient ECNU catalyst, which exhibits the highest Faraday efficiency of 60.11 % and urea yield rate of 35.80 mmol h⁻¹ g⁻¹ in flow cell. Atomic characterizations reveal that W single atoms exist as isolated W₁-S₃ moieties on MoS₂. Combined theoretical calculations and operando spectroscopic measurements demonstrate that the enhanced ECNU performance of W₁/MoS₂ arises from the construction of W₁-S₃ moieties that can promote CN coupling and hydrogenation energetics, whilst suppressing the competing side reactions.

将二氧化碳和二氧化氮电还原为尿素（ECNU）为同时迁移污染的二氧化氮和生产高附加值尿素提供了一种令人着迷的方法。本研究将原子分散在 MoS2（W1/MoS2）上的 W 设计为一种高效的 ECNU 催化剂，在流动池中表现出最高的法拉第效率（60.11%）和尿素产率（35.80 mmol h-1 g-1）。原子表征显示，W 单原子在 MoS2 上以孤立的 W1-S3 分子形式存在。综合理论计算和操作光谱测量结果表明，W1/MoS2 的 ECNU 性能增强源于 W1-S3 分子的构建，它可以促进 CN 偶联和氢化能量，同时抑制竞争性的副反应。

引用次数: 0

High-efficiency electrocatalytic hydrogen evolution in NiCo-Mo2C tandem nanoreactors with bimetallic modulation and crystal plane synergy 具有双金属调制和晶面协同作用的 NiCo-Mo2C 串联纳米反应器中的高效电催化氢气进化。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.074

Xin Chen , Aihua Jiang , Xiu Cao , Simin Tao , Lingling Chen , Hongyu Liu , Laijun Liu , Xinyu Li , Jianrong Xiao

Mo₂C, with an electronic structure closely resembling that of Pt, holds significant promise as a catalyst for nonprecious metal-based electrocatalytic hydrogen evolution reactions (HER). This study presents the design and synthesis of Ni and Co bimetallic-doped Mo₂C (NiCo-Mo₂C) tandem nanoreactors, engineered by leveraging the concept of a high-gain transistor cascade amplifier. In NiCo-Mo₂C material, each monomer layer on Mo₂C rod functions as an individual electrocatalytic nanoreactor, with the rod supporting a tandem configuration of these units. The combined modulation of Ni and Co at NiCo-Mo₂C interface increases the electron cloud density around Mo and shifts the d-band center negatively, effectively reducing Mo–H* binding energy. The synergy between NiCo-Mo₂C (1 0 1) and (0 0 2) crystal planes facilitates both water dissociation and H* desorption from Mo sites. This tandem configuration of multicatalytic units achieves enhanced hydrogen evolution, demonstrated by the low overpotential at 10 mA·cm⁻² (η₁₀) values of 129 mV and 180 mV and Tafel slopes of 84 mV·dec⁻¹ and 85 mV·dec⁻¹ in 1 M KOH and 0.5 M H₂SO₄, respectively. Through bimetallic modulation, crystal plane synergy, and tandem structuring, this work advances a novel approach to optimizing HER kinetics, presenting a valuable strategy for developing highly efficient, nonprecious metal-based electrocatalysts.

Mo2C 的电子结构与铂的电子结构非常相似，有望成为非贵金属电催化氢进化反应 (HER) 的催化剂。本研究利用高增益晶体管级联放大器的概念，设计并合成了镍和钴双金属掺杂的 Mo2C（NiCo-Mo2C）串联纳米反应器。在 NiCo-Mo2C 材料中，Mo2C 棒上的每个单体层都是一个独立的电催化纳米反应器，棒支持这些单元的串联配置。NiCo-Mo2C 界面上 Ni 和 Co 的联合调制增加了 Mo 周围的电子云密度，并使 d 带中心负向移动，从而有效降低了 Mo-H* 的结合能。NiCo-Mo2C（101）和（002）晶面之间的协同作用促进了水的解离和 Mo 位点上 H* 的解吸。在 1 M KOH 和 0.5 M H2SO4 中，10 mA-cm-2 (η10) 的低过电位值分别为 129 mV 和 180 mV，Tafel 斜率分别为 84 mV-dec-1 和 85 mV-dec-1，这表明这种串联配置的多催化单元实现了更强的氢进化能力。通过双金属调制、晶面协同作用和串联结构，这项研究提出了一种优化 HER 动力学的新方法，为开发高效的非贵金属电催化剂提供了一种宝贵的策略。

{"title":"High-efficiency electrocatalytic hydrogen evolution in NiCo-Mo2C tandem nanoreactors with bimetallic modulation and crystal plane synergy","authors":"Xin Chen , Aihua Jiang , Xiu Cao , Simin Tao , Lingling Chen , Hongyu Liu , Laijun Liu , Xinyu Li , Jianrong Xiao","doi":"10.1016/j.jcis.2024.11.074","DOIUrl":"10.1016/j.jcis.2024.11.074","url":null,"abstract":"<div><div>Mo2C, with an electronic structure closely resembling that of Pt, holds significant promise as a catalyst for nonprecious metal-based electrocatalytic hydrogen evolution reactions (HER). This study presents the design and synthesis of Ni and Co bimetallic-doped Mo2C (NiCo-Mo2C) tandem nanoreactors, engineered by leveraging the concept of a high-gain transistor cascade amplifier. In NiCo-Mo2C material, each monomer layer on Mo2C rod functions as an individual electrocatalytic nanoreactor, with the rod supporting a tandem configuration of these units. The combined modulation of Ni and Co at NiCo-Mo2C interface increases the electron cloud density around Mo and shifts the d-band center negatively, effectively reducing Mo–H* binding energy. The synergy between NiCo-Mo2C (101) and (002) crystal planes facilitates both water dissociation and H* desorption from Mo sites. This tandem configuration of multicatalytic units achieves enhanced hydrogen evolution, demonstrated by the low overpotential at 10 mA·cm−2 (η10) values of 129 mV and 180 mV and Tafel slopes of 84 mV·dec−1 and 85 mV·dec−1 in 1 M KOH and 0.5 M H2SO4, respectively. Through bimetallic modulation, crystal plane synergy, and tandem structuring, this work advances a novel approach to optimizing HER kinetics, presenting a valuable strategy for developing highly efficient, nonprecious metal-based electrocatalysts.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 53-65"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142645961","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}

引用次数: 0

Ultra-highly conductive optoelectronic modulated single-molecule nickel bis(dithiolene) junctions with strong molecule-electrode coupling 具有强分子-电极耦合的超高导电性光电调制单分子双(二硫环戊烯)镍结

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.085

Yiming Chen , Xinwei Wang , Xijuan Wang , Xinhuan Zhang , Chuanxiang Chen , Saisai Yuan , Ping Duan , Jin Li

Strong molecule-electrode coupling originating from orbit hybridization between gold and the delocalized molecular wires in single-molecule junctions facilitates facile transport towards smart molecular devices. In this paper, we report ultra-highly conductive single-molecule circuits based on highly delocalized nickel bis(dithiolene) (NiS₄) molecular junctions using scanning tunneling microscope break junction technique. Single-molecule charge transport measurement of both NiS₄ reveals they exhibits high conductance of 10^−1.49 G₀ and 10^−1.51 G₀, respectively. Moreover, under intervention of high bias voltage the molecular conductance could be further improved to approximately 10^−1.00 G₀, the highest value reported to date with similar molecular lengths. Theoretical calculations suggest that the strong hybridization of the π-channels and the gold electrodes in both junctions exists and it further extends from molecule-electrode interfaces to metal electrodes as visualized by the isosurface plots of the transmitting eigenstate, which lead to not only a distinct energy shift of the dominated LUMO peaks toward Fermi level, but also broad peaks in the LUMO resonance in the transmission functions. In addition, the both molecular junctions show remarkable photoconductance of approximately 10^−1.00 G₀ under resonant light excitation, due to possible exciton binding in these junctions. Interestingly, the conductance switching of both molecular junctions under optoelectronic modulation is highly reversible, forming a multi-stimulus responsive molecular switch. This work not only provides a building block for fabricating highly conducting molecular wires with strong molecule-electrode coupling, but also lays a foundation for designing optoelectronic modulated functional molecule-scale devices.

单分子结中的金与脱局域分子线之间的轨道杂化产生的强分子-电极耦合促进了智能分子设备的便捷传输。在本文中，我们利用扫描隧道显微镜断点技术，报告了基于高度去局域化的双(二硫环戊烯)镍（NiS4）分子结的超高导电单分子电路。对这两种 NiS4 的单分子电荷传输测量显示，它们分别表现出 10-1.49 G0 和 10-1.51 G0 的高电导率。此外，在高偏置电压的干预下，分子电导率可进一步提高到约 10-1.00 G0，这是迄今为止在类似分子长度条件下报告的最高值。理论计算表明，这两个结中的π通道和金电极之间存在着强烈的杂化作用，而且这种杂化作用从分子-电极界面进一步延伸到金属电极，这一点从透射特征状态的等值面图中可以看出，这不仅导致占主导地位的 LUMO 峰向费米级发生明显的能量移动，而且还导致透射函数中的 LUMO 共振出现宽阔的峰值。此外，在共振光激发下，这两个分子结都显示出显著的光电导性，约为 10-1.00 G0，这是由于这些分子结中可能存在激子结合。有趣的是，这两个分子结在光电调制下的电导切换是高度可逆的，从而形成了一个多刺激响应分子开关。这项工作不仅为制造具有强分子-电极耦合的高导电分子线提供了构件，还为设计光电调制功能分子级器件奠定了基础。

{"title":"Ultra-highly conductive optoelectronic modulated single-molecule nickel bis(dithiolene) junctions with strong molecule-electrode coupling","authors":"Yiming Chen , Xinwei Wang , Xijuan Wang , Xinhuan Zhang , Chuanxiang Chen , Saisai Yuan , Ping Duan , Jin Li","doi":"10.1016/j.jcis.2024.11.085","DOIUrl":"10.1016/j.jcis.2024.11.085","url":null,"abstract":"<div><div>Strong molecule-electrode coupling originating from orbit hybridization between gold and the delocalized molecular wires in single-molecule junctions facilitates facile transport towards smart molecular devices. In this paper, we report ultra-highly conductive single-molecule circuits based on highly delocalized nickel bis(dithiolene) (NiS4) molecular junctions using scanning tunneling microscope break junction technique. Single-molecule charge transport measurement of both NiS4 reveals they exhibits high conductance of 10−1.49 G0 and 10−1.51 G0, respectively. Moreover, under intervention of high bias voltage the molecular conductance could be further improved to approximately 10−1.00 G0, the highest value reported to date with similar molecular lengths. Theoretical calculations suggest that the strong hybridization of the π-channels and the gold electrodes in both junctions exists and it further extends from molecule-electrode interfaces to metal electrodes as visualized by the isosurface plots of the transmitting eigenstate, which lead to not only a distinct energy shift of the dominated LUMO peaks toward Fermi level, but also broad peaks in the LUMO resonance in the transmission functions. In addition, the both molecular junctions show remarkable photoconductance of approximately 10−1.00 G0 under resonant light excitation, due to possible exciton binding in these junctions. Interestingly, the conductance switching of both molecular junctions under optoelectronic modulation is highly reversible, forming a multi-stimulus responsive molecular switch. This work not only provides a building block for fabricating highly conducting molecular wires with strong molecule-electrode coupling, but also lays a foundation for designing optoelectronic modulated functional molecule-scale devices.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 96-104"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142653258","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}

引用次数: 0

A soft electronic skin simulating the multi-scale human touch for the detection of fruit freshness 用于检测水果新鲜度的模拟多尺度人体触感的柔软电子皮肤。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.084

Xiaoya Wei , Jing Tian , Cong Wang , Sheng Cheng , Xu Fei , Fawen Yin , Longquan Xu , Yao Li

Realizing biomimicry for human tactile perception is a meaningful challenge. In this work, a soft matter system with multi-scale energy dissipation structure is designed to realize flexible sensing and detection by biomimetic human touch. At the molecular scale, the supramolecular interactions are introduced into the hydrogel system, including the hydrophobic interaction and the ion attraction between macromolecular segments. At the micron scale, a system of “button” permeable macromolecules is constructed to absorb external forces and store energy through the sliding of macromolecules inside the “button”. By adjusting the molecular scale and micron scale structure, the obtained hydrogels demonstrate excellent mechanical properties, electrical conductivity and response sensitivity. This novel hydrogel withstands 200 compression cycles without creep deformation and outputs a stable response signal in terms of compression cycles with the signal volatility of around 1 %. Based on its good durability, this hydrogel, which simulates human multi-scale tactility, has outstanding application potential in detecting fruit damage that is difficult to observe. Notably, the construction of this multi-scale energy dissipation structure is universal for increasing the mechanical property of ACG hydrogels. The high-strength hydrogels adjusted by this strategy is significantly toughened, and the mechanical properties increased by 38 %. This work is of guiding significance for the preparation of high-performance hydrogels.

实现仿生人类触觉感知是一项有意义的挑战。本研究设计了一种具有多尺度耗能结构的软物质系统，以实现仿生人体触觉的柔性传感和检测。在分子尺度上，水凝胶系统引入了超分子相互作用，包括疏水相互作用和大分子片段之间的离子吸引力。在微米尺度上，构建了一个 "纽扣 "渗透大分子系统，通过大分子在 "纽扣 "内的滑动来吸收外力和储存能量。通过调整分子尺度和微米尺度的结构，获得的水凝胶显示出优异的机械性能、导电性和反应灵敏度。这种新型水凝胶可经受 200 次压缩循环而不发生蠕变变形，并在压缩循环中输出稳定的响应信号，信号波动率约为 1%。基于其良好的耐久性，这种模拟人体多尺度触感的水凝胶在检测难以观察到的水果损伤方面具有突出的应用潜力。值得注意的是，这种多尺度消能结构的构造对于提高 ACG 水凝胶的机械性能具有普遍意义。通过这种策略调整的高强度水凝胶具有明显的韧性，力学性能提高了 38%。这项工作对制备高性能水凝胶具有指导意义。

{"title":"A soft electronic skin simulating the multi-scale human touch for the detection of fruit freshness","authors":"Xiaoya Wei , Jing Tian , Cong Wang , Sheng Cheng , Xu Fei , Fawen Yin , Longquan Xu , Yao Li","doi":"10.1016/j.jcis.2024.11.084","DOIUrl":"10.1016/j.jcis.2024.11.084","url":null,"abstract":"<div><div>Realizing biomimicry for human tactile perception is a meaningful challenge. In this work, a soft matter system with multi-scale energy dissipation structure is designed to realize flexible sensing and detection by biomimetic human touch. At the molecular scale, the supramolecular interactions are introduced into the hydrogel system, including the hydrophobic interaction and the ion attraction between macromolecular segments. At the micron scale, a system of “button” permeable macromolecules is constructed to absorb external forces and store energy through the sliding of macromolecules inside the “button”. By adjusting the molecular scale and micron scale structure, the obtained hydrogels demonstrate excellent mechanical properties, electrical conductivity and response sensitivity. This novel hydrogel withstands 200 compression cycles without creep deformation and outputs a stable response signal in terms of compression cycles with the signal volatility of around 1 %. Based on its good durability, this hydrogel, which simulates human multi-scale tactility, has outstanding application potential in detecting fruit damage that is difficult to observe. Notably, the construction of this multi-scale energy dissipation structure is universal for increasing the mechanical property of ACG hydrogels. The high-strength hydrogels adjusted by this strategy is significantly toughened, and the mechanical properties increased by 38 %. This work is of guiding significance for the preparation of high-performance hydrogels.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 66-76"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646040","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}

引用次数: 0

Multifunctional aramid-based composite quasi-solid-state electrolytes for flexible structure batteries 用于柔性结构电池的多功能芳纶基复合准固态电解质。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.071

Wenjie He , Zhigang Li , JingZeng Gu , Gang Qin , Jia Yang , Xinxin Cao , Min Zhang , Jiangmin Jiang

The integration of flexible structure batteries (FSBs) into electronic equipment is an effective method to significantly improve energy efficiency, whereas traditional battery separators, with poor mechanical properties, low liquid electrolyte capture ability, and weak thermal stability, cannot meet the practical requirements of various applications. To address these challenges, in this study, a multifunctional composite quasi-solid-state electrolyte (CQE) was synthesized by electrospinning poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) fibers on both sides of an aramid nanofibers (ANFs) fibrous film for application in high-performance FSBs. Here, the ANF film serves as a structural framework, thus enhancing the mechanical properties and thermal stability of the CQE, while the “thermal closed-hole effect” and liquid electrolyte capture capability of the PVDF-HFP film in the CQE improve the overall safety of the FSBs. The design strategy of combining 3D-printed electrodes and functional CQE is essential to achieving the integration of structural support and energy storage. Due to the unique characteristics of the CQE, the assembled full-battery (LiFePO₄//Li₄Ti₅O₁₂) demonstrates superior cycling stability (500 cycles). The assembled rectangular bag battery was also shown to be capable of powering an LED lamp under bending conditions and external force, thus providing valuable insights into FSBs design in the field of energy storage.

将柔性结构电池（FSB）集成到电子设备中是大幅提高能效的有效方法，而传统的电池隔膜机械性能差、液态电解质捕获能力低、热稳定性弱，无法满足各种应用的实际要求。为了应对这些挑战，本研究在芳纶纳米纤维（ANFs）纤维膜的两侧电纺丝聚偏二氟乙烯-六氟丙烯（PVDF-HFP）纤维，合成了一种多功能复合准固态电解质（CQE），用于高性能 FSB。在这里，ANF 薄膜可作为结构框架，从而增强 CQE 的机械性能和热稳定性，而 CQE 中 PVDF-HFP 薄膜的 "热闭孔效应 "和液态电解质捕获能力则提高了 FSB 的整体安全性。将 3D 打印电极和功能性 CQE 相结合的设计策略对于实现结构支撑和能量存储的一体化至关重要。由于 CQE 的独特特性，组装后的全电池（LiFePO4//Li4Ti5O12）显示出卓越的循环稳定性（500 次循环）。组装好的矩形袋电池还能在弯曲条件和外力作用下为 LED 灯供电，从而为储能领域的 FSB 设计提供了宝贵的启示。

{"title":"Multifunctional aramid-based composite quasi-solid-state electrolytes for flexible structure batteries","authors":"Wenjie He , Zhigang Li , JingZeng Gu , Gang Qin , Jia Yang , Xinxin Cao , Min Zhang , Jiangmin Jiang","doi":"10.1016/j.jcis.2024.11.071","DOIUrl":"10.1016/j.jcis.2024.11.071","url":null,"abstract":"<div><div>The integration of flexible structure batteries (FSBs) into electronic equipment is an effective method to significantly improve energy efficiency, whereas traditional battery separators, with poor mechanical properties, low liquid electrolyte capture ability, and weak thermal stability, cannot meet the practical requirements of various applications. To address these challenges, in this study, a multifunctional composite quasi-solid-state electrolyte (CQE) was synthesized by electrospinning poly(vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) fibers on both sides of an aramid nanofibers (ANFs) fibrous film for application in high-performance FSBs. Here, the ANF film serves as a structural framework, thus enhancing the mechanical properties and thermal stability of the CQE, while the “thermal closed-hole effect” and liquid electrolyte capture capability of the PVDF-HFP film in the CQE improve the overall safety of the FSBs. The design strategy of combining 3D-printed electrodes and functional CQE is essential to achieving the integration of structural support and energy storage. Due to the unique characteristics of the CQE, the assembled full-battery (LiFePO4//Li4Ti5O12) demonstrates superior cycling stability (500 cycles). The assembled rectangular bag battery was also shown to be capable of powering an LED lamp under bending conditions and external force, thus providing valuable insights into FSBs design in the field of energy storage.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 77-84"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646001","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}

引用次数: 0

Construction of directional electron transfer from Pt to MoO2-x in macroporous structure for efficient hydrogen oxidation 在大孔结构中构建从 Pt 到 MoO2-x 的定向电子转移，以实现高效氢氧化。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.073

Rundong Ma , Han Tian , Xu Yu , Xiangzhi Cui , Xinmei Hou , Shengli An

Hydrogen oxidation reaction (HOR) as the anode reaction in proton exchange membrane fuel cell, usually suffers from the high loading of platinum (Pt) and subsequent CO poisoning especially by using industrial crude hydrogen as fuel. In this work, we propose a directional electron transfer route from Pt to MoO_2-_x in the macroporous structure to significantly enhance the HOR activity as well as the CO tolerance, which is constructed by interface engineering and defect strategy to anchor highly dispersed Pt nanoparticles onto the three-dimensional MoO_2-_x-C framework. The optimized 2Pt-MoO_2-_x-C with 1.02 wt% Pt demonstrates higher HOR peak current density (3.57 mA cm⁻²) and nearly 25 times higher mass activity than 20 wt% Pt/C. The excellent HOR performance is attributed to the synergistic effect between Pt and MoO_2-_x species, in which the charge transfer from Pt to MoO_2-_x improves H₂ adsorption ability of Pt and accelerates the activation of H₂ due to the reduced hydrogen binding energy of MoO_2-_x caused by Pt-O construction, leading to the release of H* thereby the enhancement of HOR activity. The construction of three-dimensional macroporous structure enhances the HOR dynamics by promoting the conductivity, mass transfer and the exposure of active sites. Moreover, the formed Mo-OH in Pt-MoO_2-_x-C can effectively react with CO species to remove the CO poisoning of Pt, endowing the excellent CO tolerance.

氢氧化反应（HOR）作为质子交换膜燃料电池中的阳极反应，通常会受到铂（Pt）负载过高以及随后一氧化碳中毒的影响，尤其是在使用工业粗氢作为燃料时。在这项工作中，我们提出了一条从铂到大孔结构中的 MoO2-x 的定向电子转移路线，通过界面工程和缺陷策略将高度分散的铂纳米粒子锚定在三维 MoO2-x-C 框架上，从而显著提高了氢氧根活性和对 CO 的耐受性。优化后的 2Pt-MoO2-x-C 与 20 wt% Pt/C 相比，铂含量为 1.02 wt%，具有更高的氢氧峰值电流密度（3.57 mA cm-2）和近 25 倍的质量活性。Pt 与 MoO2-x 之间的电荷转移提高了 Pt 对 H2 的吸附能力，同时由于 Pt-O 构建降低了 MoO2-x 的氢结合能，加速了 H2 的活化，导致 H* 的释放，从而提高了 HOR 活性。三维大孔结构的构建促进了传导、传质和活性位点的暴露，从而增强了 HOR 的活性。此外，Pt-MoO2-x-C 中形成的 Mo-OH 能有效地与 CO 物种发生反应，消除 CO 对铂的毒害，从而赋予铂优异的 CO 耐受性。

{"title":"Construction of directional electron transfer from Pt to MoO2-x in macroporous structure for efficient hydrogen oxidation","authors":"Rundong Ma , Han Tian , Xu Yu , Xiangzhi Cui , Xinmei Hou , Shengli An","doi":"10.1016/j.jcis.2024.11.073","DOIUrl":"10.1016/j.jcis.2024.11.073","url":null,"abstract":"<div><div>Hydrogen oxidation reaction (HOR) as the anode reaction in proton exchange membrane fuel cell, usually suffers from the high loading of platinum (Pt) and subsequent CO poisoning especially by using industrial crude hydrogen as fuel. In this work, we propose a directional electron transfer route from Pt to MoO2-x in the macroporous structure to significantly enhance the HOR activity as well as the CO tolerance, which is constructed by interface engineering and defect strategy to anchor highly dispersed Pt nanoparticles onto the three-dimensional MoO2-x-C framework. The optimized 2Pt-MoO2-x-C with 1.02 wt% Pt demonstrates higher HOR peak current density (3.57 mA cm−2) and nearly 25 times higher mass activity than 20 wt% Pt/C. The excellent HOR performance is attributed to the synergistic effect between Pt and MoO2-x species, in which the charge transfer from Pt to MoO2-x improves H2 adsorption ability of Pt and accelerates the activation of H2 due to the reduced hydrogen binding energy of MoO2-x caused by Pt-O construction, leading to the release of H* thereby the enhancement of HOR activity. The construction of three-dimensional macroporous structure enhances the HOR dynamics by promoting the conductivity, mass transfer and the exposure of active sites. Moreover, the formed Mo-OH in Pt-MoO2-x-C can effectively react with CO species to remove the CO poisoning of Pt, endowing the excellent CO tolerance.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 1-10"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643654","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}

引用次数: 0

Enhanced dielectric performances of strontium barium titanate nanorod composites via improved interfacial compatibility 通过改善界面相容性提高钛酸锶钡纳米棒复合材料的介电性能。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-14 DOI: 10.1016/j.jcis.2024.11.088

Yongxian Liu , Bo Tang , Zaixing Wang , Yayao Jiao , Qingqing Hou , Zhangting Dang , Xiufu Hua , Liping Wei , Lingling Wang , Renbo Wei

High performance film capacitor has attracted widespread attention due to their increasing applications in electronic devices. However, the insufficient dielectric properties of dielectrics in capacitors severely restrict their practical application. In this work, the dielectric performances of polyarylene ether nitrile (PEN) are effectively enhanced by the synthesizing and employing of carboxylated PEN (CPEN) modified one-dimensional (1D) strontium barium titanate nanorod (BSTNR) (CPEN@BSTNR), as well as applying of hot stretching technique. CPEN@BSTNR is prepared via the synthesizing of BSTNR, modifying with γ-Aminopropyl triethoxysilane (KH550), and grafting by CPEN. Deriving from the 1D structure of BSTNR and the peripheral modification by CPEN, compatibility of CPEN@BSTNR in PEN has been significantly improved. Moreover, CPEN@BSTNR orients in the polymer matrix attributing to the hot stretching. Consequently, the hot stretched 16 wt% CPEN@BSTNR/PEN film exhibits an increased dielectric constant of 17.30 and maintained a breakdown strength of 204.1 kV/mm. As a result, this stretched composite film demonstrates an energy density up to 3.19 J/cm³, with a 300 % improvement over pure PEN. This enhanced dielectric properties of PEN presents a promising avenue for the fabrication of high performance film capacitors.

高性能薄膜电容器在电子设备中的应用日益广泛，因而受到了广泛关注。然而，电容器电介质性能的不足严重限制了其实际应用。在这项研究中，通过合成和使用羧基化聚丙烯（CPEN）修饰的一维（1D）钛酸锶钡纳米棒（BSTNR）（CPEN@BSTNR），并应用热拉伸技术，有效地提高了聚芳醚腈（PEN）的介电性能。CPEN@BSTNR 的制备方法是合成 BSTNR，用γ-氨基丙基三乙氧基硅烷（KH550）改性，再用 CPEN 接枝。基于 BSTNR 的一维结构和 CPEN 的外围修饰，CPEN@BSTNR 在 PEN 中的相容性得到了显著改善。此外，CPEN@BSTNR 在聚合物基体中的定向归功于热拉伸。因此，热拉伸 16 wt% CPEN@BSTNR/PEN 薄膜的介电常数增加到 17.30，击穿强度保持在 204.1 kV/mm。因此，这种拉伸复合薄膜的能量密度高达 3.19 J/cm3，比纯 PEN 提高了 300%。PEN 介电特性的增强为制造高性能薄膜电容器提供了一条前景广阔的途径。

{"title":"Enhanced dielectric performances of strontium barium titanate nanorod composites via improved interfacial compatibility","authors":"Yongxian Liu , Bo Tang , Zaixing Wang , Yayao Jiao , Qingqing Hou , Zhangting Dang , Xiufu Hua , Liping Wei , Lingling Wang , Renbo Wei","doi":"10.1016/j.jcis.2024.11.088","DOIUrl":"10.1016/j.jcis.2024.11.088","url":null,"abstract":"<div><div>High performance film capacitor has attracted widespread attention due to their increasing applications in electronic devices. However, the insufficient dielectric properties of dielectrics in capacitors severely restrict their practical application. In this work, the dielectric performances of polyarylene ether nitrile (PEN) are effectively enhanced by the synthesizing and employing of carboxylated PEN (CPEN) modified one-dimensional (1D) strontium barium titanate nanorod (BSTNR) (CPEN@BSTNR), as well as applying of hot stretching technique. CPEN@BSTNR is prepared via the synthesizing of BSTNR, modifying with γ-Aminopropyl triethoxysilane (KH550), and grafting by CPEN. Deriving from the 1D structure of BSTNR and the peripheral modification by CPEN, compatibility of CPEN@BSTNR in PEN has been significantly improved. Moreover, CPEN@BSTNR orients in the polymer matrix attributing to the hot stretching. Consequently, the hot stretched 16 wt% CPEN@BSTNR/PEN film exhibits an increased dielectric constant of 17.30 and maintained a breakdown strength of 204.1 kV/mm. As a result, this stretched composite film demonstrates an energy density up to 3.19 J/cm3, with a 300 % improvement over pure PEN. This enhanced dielectric properties of PEN presents a promising avenue for the fabrication of high performance film capacitors.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 85-95"},"PeriodicalIF":9.4,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142645956","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}

引用次数: 0

Cr-doped NiFe sulfides nanoplate array: Highly efficient and robust bifunctional electrocatalyst for the overall water splitting and seawater electrolysis 掺杂铬的镍铁硫化物纳米板阵列：用于整体水分离和海水电解的高效、稳健的双功能电催化剂。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-13 DOI: 10.1016/j.jcis.2024.11.072

Yujia He , Xuan Yang , Mingyuan Jiang , Fuguang Liu , Jinming Zhang , Huiying Li , Liang Cui , Jiangtao Xu , Xuqiang Ji , Jingquan Liu

To replace precious metals and reduce production costs for large-scale hydrogen production, developing stable, high-performance transition metal electrocatalysts that can be used in a wide range of environments is desirable yet challenging. Herein, a self-supported hybrid catalyst (NiFeCrS_x/NF) with high electrocatalytic activity was designed and constructed using conductive nickel foam as a substrate via manipulation of the cation doping ratio of transition metal compounds. Due to the strong coupling synergy between the metal sulfides NiS₂, Fe₉S₁₁, and Cr₂S₃, as well as their interaction with the conductive nickel foam (NF), the energy barrier for catalytic reactions is reduced, and the charge transfer rate is enhanced. This significantly improves the hydrogen evolution reaction (HER) performance of NiFeCrS_x/NF, achieving a current density of 10 mA cm⁻² with an overpotential of just 66 mV. Furthermore, doping with chromium generates different valence states of Cr during the catalytic process, which can synergize with the high-valent Fe and Ni, promoting the formation of oxygen vacancies and enriching the active sites for the oxygen evolution reaction (OER). Consequently, at a current density of 10 mA cm⁻² in 1.0 M KOH, the overpotential for OER is only 223 mV for NiFeCrS_x/NF. Additionally, the in situ grown of self-supporting nanoflower structure on NiFe-LDH not only provides a large catalytic surface area but also facilitates electrolyte penetration during the catalytic process, endowing NiFeCrS_x/NF with high long-term stability. When used as a bifunctional catalyst for overall water splitting, the NiFeCrS_x/NF||NiFeCrS_x/NF electrolyzer requires only 1.29 V to deliver a current density of 10 mA cm⁻². Simultaneously, Cr doping protects the Fe sites by maintaining stable valence states, ensuring high performance and stability of NiFeCrS_x/NF, even when it is utilized for seawater splitting. This strategy offers novel concepts for creating catalysts based on non-precious metals that can be utilized in various application scenarios.

为了取代贵金属并降低大规模制氢的生产成本，开发可在多种环境中使用的稳定、高性能过渡金属电催化剂是非常理想的，但也是极具挑战性的。在此，通过操纵过渡金属化合物的阳离子掺杂比例，设计并构建了一种以导电泡沫镍为基底的具有高电催化活性的自支撑混合催化剂（NiFeCrSx/NF）。由于金属硫化物 NiS2、Fe9S11 和 Cr2S3 之间的强耦合协同作用，以及它们与导电泡沫镍（NF）之间的相互作用，降低了催化反应的能量势垒，提高了电荷转移速率。这大大提高了 NiFeCrSx/NF 的氢进化反应（HER）性能，使其电流密度达到 10 mA cm-2，过电位仅为 66 mV。此外，在催化过程中，铬的掺杂会产生不同价态的铬，与高价的铁和镍协同作用，促进氧空位的形成，丰富氧进化反应（OER）的活性位点。因此，在 1.0 M KOH 中，当电流密度为 10 mA cm-2 时，NiFeCrSx/NF 的氧进化反应过电位仅为 223 mV。此外，NiFe-LDH 上原位生长的自支撑纳米花结构不仅提供了较大的催化表面积，还有利于催化过程中电解质的渗透，从而使 NiFeCrSx/NF 具有较高的长期稳定性。当用作整体水分离的双功能催化剂时，NiFeCrSx/NF||NiFeCrSx/NF 电解槽只需要 1.29 V 的电压就能提供 10 mA cm-2 的电流密度。同时，铬的掺杂通过保持稳定的价态来保护铁的位点，从而确保了 NiFeCrSx/NF 的高性能和稳定性，即使将其用于海水分离也是如此。这种策略为创造基于非贵金属的催化剂提供了新的概念，这种催化剂可用于各种应用场合。

{"title":"Cr-doped NiFe sulfides nanoplate array: Highly efficient and robust bifunctional electrocatalyst for the overall water splitting and seawater electrolysis","authors":"Yujia He , Xuan Yang , Mingyuan Jiang , Fuguang Liu , Jinming Zhang , Huiying Li , Liang Cui , Jiangtao Xu , Xuqiang Ji , Jingquan Liu","doi":"10.1016/j.jcis.2024.11.072","DOIUrl":"10.1016/j.jcis.2024.11.072","url":null,"abstract":"<div><div>To replace precious metals and reduce production costs for large-scale hydrogen production, developing stable, high-performance transition metal electrocatalysts that can be used in a wide range of environments is desirable yet challenging. Herein, a self-supported hybrid catalyst (NiFeCrSx/NF) with high electrocatalytic activity was designed and constructed using conductive nickel foam as a substrate via manipulation of the cation doping ratio of transition metal compounds. Due to the strong coupling synergy between the metal sulfides NiS2, Fe9S11, and Cr2S3, as well as their interaction with the conductive nickel foam (NF), the energy barrier for catalytic reactions is reduced, and the charge transfer rate is enhanced. This significantly improves the hydrogen evolution reaction (HER) performance of NiFeCrSx/NF, achieving a current density of 10 mA cm−2 with an overpotential of just 66 mV. Furthermore, doping with chromium generates different valence states of Cr during the catalytic process, which can synergize with the high-valent Fe and Ni, promoting the formation of oxygen vacancies and enriching the active sites for the oxygen evolution reaction (OER). Consequently, at a current density of 10 mA cm−2 in 1.0 M KOH, the overpotential for OER is only 223 mV for NiFeCrSx/NF. Additionally, the in situ grown of self-supporting nanoflower structure on NiFe-LDH not only provides a large catalytic surface area but also facilitates electrolyte penetration during the catalytic process, endowing NiFeCrSx/NF with high long-term stability. When used as a bifunctional catalyst for overall water splitting, the NiFeCrSx/NF||NiFeCrSx/NF electrolyzer requires only 1.29 V to deliver a current density of 10 mA cm−2. Simultaneously, Cr doping protects the Fe sites by maintaining stable valence states, ensuring high performance and stability of NiFeCrSx/NF, even when it is utilized for seawater splitting. This strategy offers novel concepts for creating catalysts based on non-precious metals that can be utilized in various application scenarios.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 1079-1089"},"PeriodicalIF":9.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646702","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}

引用次数: 0

Enhanced photoelectric desalination of Co3O4@NC/BiVO4 photoanode via in-situ construction of hole transport layer 通过原位构建空穴传输层增强 Co3O4@NC/BiVO4 光阳极的光电脱盐能力。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-11-13 DOI: 10.1016/j.jcis.2024.11.081

Jianrong Li , Shengbo Yuan , Xueling Zhang , Fuming Chen , Yang Yang , Jian Kang , Yan He , Jinlong Han , Xiaoman Li , Yongqing Yang , Min Luo

The solar-driven photoelectrochemical desalination (SD-PED) technology, as a new emerging desalination technique, has been developed and attracted the increasing attention. However, practical application remains hampered by several constraints, including the rapid deterioration of photocurrent, and the long-term stability of system. In this research, MOF-derived nitrogen-doped carbon@Co₃O₄/BVO (Co₃O₄@NC/BVO) heterostructured photoanode was design for efficient and durable solar driven redox desalination. It exhibits an initial photocurrent of 2.40 mA/cm² and a desalination rate of 69.01 μg/(cm²·min) in the zero-bias state using the light as the driving force, without consuming electrical energy. Furthermore, the solar energy consumption of the photoanode is 0.187 μmol/J. The salt removal rate fluctuates within 1.36 μg/(cm²·min) throughout five cycles without any substantial decrease. Photo-luminescence, EIS and Mott-Schottky analysis are also performed to investigate interface reaction, charge separation and transfer mechanism between photoanode and electrolyte. The analysis of the charge-transfer paths on the heterojunction interface is conducted through in situ irradiation XPS. Further analysis of the generation and separation of •OH and h⁺ in the Co₃O₄@NC/BVO photoanode using electron paramagnetic resonance (EPR) showed that Co₃O₄@NC as an efficient hole transfer layer can effectively promote the separation and transfer of photo-generated electrons and holes. The excellent desalination performance is attributed to the synergistic effect of electron transfer in the Co₃O₄@NC/BVO heterojunction and hole transport in the Co₃O₄@NC efficient hole transport layer. This work is significant for the development of solar redox flow desalination.

太阳能驱动的光电化学海水淡化（SD-PED）技术作为一种新兴的海水淡化技术，已经得到开发并引起越来越多的关注。然而，光电流的快速衰减和系统的长期稳定性等制约因素仍然阻碍着该技术的实际应用。本研究设计了氮掺杂 MOF 衍生碳@Co3O4/BVO（Co3O4@NC/BVO）异质结构光阳极，用于高效、持久的太阳能驱动氧化还原海水淡化。它的初始光电流为 2.40 mA/cm2，在以光为驱动力的零偏压状态下，脱盐率为 69.01 μg/（cm2-min），且不消耗电能。此外，光阳极的太阳能消耗量为 0.187 μmol/J。在五个周期内，盐分去除率在 1.36 μg/（cm2-min）的范围内波动，没有大幅下降。此外，还进行了光致发光、EIS 和 Mott-Schottky 分析，以研究光阳极与电解质之间的界面反应、电荷分离和转移机制。通过原位照射 XPS 分析了异质结界面上的电荷转移路径。利用电子顺磁共振（EPR）进一步分析了 Co3O4@NC/BVO 光阳极中 -OH 和 h+ 的产生和分离，结果表明 Co3O4@NC 作为高效的空穴传输层能有效促进光生电子和空穴的分离和传输。优异的海水淡化性能归功于 Co3O4@NC/BVO 异质结中电子转移和 Co3O4@NC 高效空穴传输层中空穴传输的协同效应。这项工作对太阳能氧化还原流海水淡化的发展具有重要意义。

{"title":"Enhanced photoelectric desalination of Co3O4@NC/BiVO4 photoanode via in-situ construction of hole transport layer","authors":"Jianrong Li , Shengbo Yuan , Xueling Zhang , Fuming Chen , Yang Yang , Jian Kang , Yan He , Jinlong Han , Xiaoman Li , Yongqing Yang , Min Luo","doi":"10.1016/j.jcis.2024.11.081","DOIUrl":"10.1016/j.jcis.2024.11.081","url":null,"abstract":"<div><div>The solar-driven photoelectrochemical desalination (SD-PED) technology, as a new emerging desalination technique, has been developed and attracted the increasing attention. However, practical application remains hampered by several constraints, including the rapid deterioration of photocurrent, and the long-term stability of system. In this research, MOF-derived nitrogen-doped carbon@Co3O4/BVO (Co3O4@NC/BVO) heterostructured photoanode was design for efficient and durable solar driven redox desalination. It exhibits an initial photocurrent of 2.40 mA/cm2 and a desalination rate of 69.01 μg/(cm2·min) in the zero-bias state using the light as the driving force, without consuming electrical energy. Furthermore, the solar energy consumption of the photoanode is 0.187 μmol/J. The salt removal rate fluctuates within 1.36 μg/(cm2·min) throughout five cycles without any substantial decrease. Photo-luminescence, EIS and Mott-Schottky analysis are also performed to investigate interface reaction, charge separation and transfer mechanism between photoanode and electrolyte. The analysis of the charge-transfer paths on the heterojunction interface is conducted through in situ irradiation XPS. Further analysis of the generation and separation of •OH and h+ in the Co3O4@NC/BVO photoanode using electron paramagnetic resonance (EPR) showed that Co3O4@NC as an efficient hole transfer layer can effectively promote the separation and transfer of photo-generated electrons and holes. The excellent desalination performance is attributed to the synergistic effect of electron transfer in the Co3O4@NC/BVO heterojunction and hole transport in the Co3O4@NC efficient hole transport layer. This work is significant for the development of solar redox flow desalination.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"680 ","pages":"Pages 11-23"},"PeriodicalIF":9.4,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142645958","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}

引用次数: 0