Journal of Colloid and Interface Science最新文献_第2页

Polymerization-induced highly brilliant and color-recordable mechanochromic photonic gels for ink-free patterning 用于无墨图案化的聚合诱导型高亮度可录色机械变色光子凝胶

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-30 DOI: 10.1016/j.jcis.2024.10.178

Mechanochromic photonic crystals (MPCs) are extremely attractive since they can adjust their structural color by forces. However, the poor color saturation and color-recordability of conventional MPCs significantly limit their practical applications. Herein, a highly brilliant and color-recordable MPC gel (MPCG) has been fabricated by photopolymerizing the liquid photonic crystals with silica particles non-closely packed in acrylate, dichlorobenzene, and oleylamine. Photopolymerization induces elastic gradient non-close-packing structures and thus broad photonic bandgaps (>100 nm), resulting in 1) high color saturation despite possessing a small refractive index contrast (0.06), 2) remarkable mechanochromic properties, including a large wavelength tuning range (228 nm), fast responsiveness (8.8–10.3 nm/ms), and high sensitivity (4.4 nm/kPa), and 3) unconventional color-recordable properties. MPCGs were experimentally proved to be ideal rewritable papers for constructing multicolor and high-resolution patterns in an ink-free way, difficult for traditional MPC-based units. The unique working mechanism of polymerization-induced phase separation and thus continuous swelling and gelation, and precise design of materials and structures are the keys to MPCGs’ characteristics. This study paves a new way for constructing advanced stimulus-responsive photonic structures and will promote their applications in printing, display, anti-counterfeiting, etc.

机械变色光子晶体（MPC）可以通过力来调整其结构颜色，因此极具吸引力。然而，传统 MPC 的色彩饱和度和色彩可记录性较差，极大地限制了其实际应用。在此，我们利用丙烯酸酯、二氯苯和油胺对液态光子晶体与非紧密包覆的二氧化硅颗粒进行光聚合，制造出了一种高亮度、可记录颜色的 MPC 凝胶（MPCG）。光聚合诱导出弹性梯度非紧密堆积结构，从而产生宽广的光子带隙（100 nm），导致：1）尽管折射率对比很小（0.06），但颜色饱和度很高；2）具有显著的机械变色特性，包括波长调节范围大（228 nm）、响应速度快（8.8-10.3 nm/ms）和灵敏度高（4.4 nm/kPa）；3）具有非常规的颜色可记录特性。实验证明，MPCG 是一种理想的可复写纸，能以无墨方式构建多色和高分辨率图案，这是传统 MPC 单元难以实现的。聚合诱导相分离进而持续溶胀和凝胶化的独特工作机制以及材料和结构的精确设计是 MPCGs 特性的关键所在。这项研究为构建先进的刺激响应型光子结构铺平了新的道路，并将促进其在印刷、显示、防伪等领域的应用。

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引用次数: 0

Co/CoTe heterostructure internal hairy fibers as high-efficiency oxygen electrocatalyst for Zn-air batteries 作为锌-空气电池高效氧气电催化剂的 Co/CoTe 异质结构内部毛状纤维

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-29 DOI: 10.1016/j.jcis.2024.10.183

The design of highly efficient catalysts to enhance the kinetics of oxygen reduction (OER) and oxygen evolution (ORR) reactions is the key issue for the development of high-performance Zn-air battery. In this work, we report the design of Co-CoTe heterostructured fibers as the bifunctional oxygen catalyst for Zn-air battery. Firstly, the theoretical analysis was carried out on Co-CoTe heterostructure. The large work function difference is favorable to construct strong interfacial built-in electric field (BIEF), and the low energy barrier endows high catalytic activities. Moreover, the in-situ grown carbon shell was designed to build “core–shell” Co-CoTe/C unit to realize its high performance. They assemble the Co-CoTe@HFS fiber with good self-supporting and flexible features. Taken the advantages of the strong BIEF, the “core–shell” basic unit, and the freestanding substrate, the Co-CoTe@HFS fiber achieves the good electrocatalytic properties and high reliability. The full Zn-air battery (ZAB) with the Co/CoTe@HFS air cathode achieves the high peak power density and cycling stability over long-term cycling. Therefore, this work provides a clue to design bifunctional oxygen catalysts for high-performance ZABs.

设计高效催化剂以提高氧还原（OER）和氧进化（ORR）反应的动力学是开发高性能锌-空气电池的关键问题。在这项工作中，我们报告了作为锌-空气电池双功能氧催化剂的 Co-CoTe 异质结构纤维的设计。首先，我们对 Co-CoTe 异质结构进行了理论分析。大功函数差有利于构建强界面内置电场（BIEF），低能垒赋予了催化活性。此外，他们还设计了原位生长的碳壳，以构建 "核壳 "Co-CoTe/C 单元，从而实现其高性能。他们组装的 Co-CoTe@HFS 纤维具有良好的自支撑性和柔韧性。Co-CoTe@HFS纤维具有良好的自承性和柔韧性，利用强BIEF、"核壳 "基本单元和独立基底的优势，实现了良好的电催化性能和高可靠性。采用 Co/CoTe@HFS 空气正极的全 Zn 空气电池（ZAB）可实现较高的峰值功率密度和长期循环稳定性。因此，这项工作为设计用于高性能 ZAB 的双功能氧催化剂提供了线索。

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引用次数: 0

Entire ultrathin two-dimensional pseudocapacitive nanosheets with high active covalent groups for flexible asymmetric all-solid-state micro-pseudocapacitors with high energy density and long cycle life 具有高活性共价基团的整片超薄二维伪电容纳米片可用于具有高能量密度和长循环寿命的柔性不对称全固态微型伪电容器。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.144

Micro-supercapacitors (MSCs) are gradually emerging as a strong contender for the next wearable and portable micro-energy storage devices. Low energy density and poor stability are significant challenges to their widespread application. Based on this, a novel asymmetric all-solid-state Micro-pseudocapacitors (AMPCs) is designed elaborately, in which all the active materials are based on conducting two-dimensional (2D) materials with thin lamellar thickness and active covalent groups on the surface. The positive electrode was made of covalently graft-modified GO with p-phenylenediamine (PrGO), while the negative electrode was made of MXene material. Besides, electrochemically exfoliated graphene (EG) was incorporated into the positive electrode to further improve the electrochemical performance of the PrGO@EG hybrid film electrode due to its excellent conductivity and favorable π-π stacking effects. As a result, the PrGO@EG-30 % electrode demonstrates a high specific capacity of 571 F cm⁻³ (411 F/g) and maintains excellent stability, retaining 100 % of its capacity even after 10,000 cycles. Surprisingly, the assembled-designed PrGO@EG//MXene AMPCs achieved remarkable electrochemical performance in solid-state electrolytes with a notable capacity of 185.4 F cm⁻³ (84.6 F/g), impressive stability with 100 % retention after 10,000 cycles, and outstanding volumetric energy density up to 50.5 μWh cm⁻³, exceeding the majorities of other state-of-the-art MSCs. Moreover, the microdevices can be easily integrated and electrochemically stable under various bending conditions, demonstrating their significant potential as flexible micro-energy storage devices.

微型超级电容器（MSC）正逐渐成为下一代可穿戴和便携式微型能量存储设备的有力竞争者。能量密度低和稳定性差是其广泛应用面临的重大挑战。基于此，我们精心设计了一种新型非对称全固态微型伪电容器（AMPCs），其中所有的活性材料都是基于导电的二维（2D）材料，具有薄层厚度和表面活性共价基团。正极由对苯二胺（PrGO）共价接枝改性的 GO 制成，负极由 MXene 材料制成。此外，正极中还加入了电化学剥离石墨烯（EG），以进一步提高 PrGO@EG 混合薄膜电极的电化学性能。因此，PrGO@EG-30 % 电极的比容量高达 571 F cm-3（411 F/g），并保持了极佳的稳定性，即使在 10,000 次循环后仍能保持 100 % 的容量。令人惊讶的是，组装设计的 PrGO@EG//MXene AMPC 在固态电解质中实现了显著的电化学性能，容量高达 185.4 F cm-3（84.6 F/g），稳定性令人印象深刻，10000 次循环后仍能保持 100%的容量，体积能量密度高达 50.5 μWh cm-3，超过了大多数其他最先进的 MSC。此外，这种微型器件易于集成，而且在各种弯曲条件下都能保持电化学稳定，这表明它们具有作为灵活微型储能器件的巨大潜力。

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引用次数: 0

A multi-functional integrated nanoplatform based on a tumor microenvironment-responsive PtAu/MnO2 cascade nanoreactor with multi-enzymatic activities for multimodal synergistic tumor therapy 基于肿瘤微环境响应型 PtAu/MnO2 级联纳米反应器的多功能集成纳米平台，具有多种酶活性，可用于多模式肿瘤协同治疗

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.160

The utilization or improvement of tumor microenvironment (TME) has become a breakthrough in emerging oncology therapies. To address the limited therapeutic efficacy of single modality, a multi-functional integrated nanoplatform based on a TME-responsive PtAu/MnO₂ cascade nanoreactor with multi-enzymatic activities was developed for multimodal synergistic tumor therapy. Benefiting from the slightly acidic environment and high-level glutathione (GSH) in TME, PtAu/MnO₂ cascade nanoreactor consumed GSH, followed by the reductive generation of manganese ion (Mn²⁺) and the release of PtAu nanoparticles (NPs). Then, the multimodal synergistic tumor therapy was activated as follows. First, GSH depletion inhibited the activity of glutathione peroxidase 4 and led to the accumulation of lipid peroxidation, thereby inducing tumor cell ferroptosis. Second, PtAu NPs exhibited catalase-like, glucose oxidase-like and nicotinamide adenine dinucleotide (NADH) oxidase-like activities, which generated oxygen for the cascade reaction to alleviate hypoxia and further depleted glucose, NADH and adenosine triphosphate, leading to the inhibition of tumor cell proliferation via starvation therapy. Third, the production of reactive oxygen species by the oxidase- and peroxidase-like activities of PtAu NPs and the Fenton-like reaction of Mn²⁺ simultaneously induced tumor cell apoptosis via chemodynamic therapy. Briefly, the in vitro and in vivo results confirmed that the multi-functional integrated nanoplatform based on a PtAu/MnO₂ cascade nanoreactor with five nanozyme activities demonstrated outstanding biocompatibility and greater inhibition of tumor growth via synergistic ferroptosis/starvation therapy/apoptosis.

利用或改善肿瘤微环境（TME）已成为新兴肿瘤疗法的一个突破口。为了解决单一疗法疗效有限的问题，我们开发了一种多功能集成纳米平台，该平台基于具有多酶活性的TME响应型PtAu/MnO2级联纳米反应器，可用于多模式协同肿瘤治疗。PtAu/MnO2级联纳米反应器利用TME中的微酸性环境和高水平谷胱甘肽（GSH），消耗GSH，然后还原生成锰离子（Mn2+）并释放PtAu纳米颗粒（NPs）。随后，多模式肿瘤协同疗法被激活。首先，GSH 的耗竭抑制了谷胱甘肽过氧化物酶 4 的活性，导致脂质过氧化物的积累，从而诱导肿瘤细胞铁中毒。其次，PtAu NPs 具有过氧化氢酶样、葡萄糖氧化酶样和烟酰胺腺嘌呤二核苷酸（NADH）氧化酶样活性，为级联反应生成氧气，缓解缺氧，并进一步耗竭葡萄糖、NADH 和三磷酸腺苷，通过饥饿疗法抑制肿瘤细胞增殖。第三，PtAu NPs 的氧化酶和过氧化物酶样活性以及 Mn2+ 的芬顿样反应产生的活性氧同时通过化学动力学疗法诱导肿瘤细胞凋亡。简而言之，体外和体内研究结果证实，基于具有五种纳米酶活性的 PtAu/MnO2 级联纳米反应器的多功能集成纳米平台具有出色的生物相容性，并能通过协同铁氧化/饥饿疗法/细胞凋亡抑制肿瘤生长。

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引用次数: 0

Synergistic effect of multi-metal site provided by Ni-N4, adjacent single metal atom, and Fe6 nanoparticle to boost CO2 activation and reduction Ni-N4、相邻单金属原子和 Fe6 纳米粒子提供的多金属位点对促进二氧化碳活化和还原的协同效应

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.166

Single transition metal (TM) atom embedded in nitrogen-doped carbon materials with M−N_x−C configuration have emerged as a promising class of electrocatalysts for electrochemical CO₂ reduction (CO₂RR). However, at high TM atom densities, a comprehensive understanding of the active site structure and reaction mechanisms remains a significant challenge, yet it is crucial for enhancing CO₂RR performance. In this work, we use first-principles calculations to investigate the electrocatalytic performance of Ni-N₄ sites for CO2 reduction to CO, co-assisted by neighboring TM atoms and a Fe₆ nanoparticle. Unlike many previously studied Ni-N₄ catalysts that maintain a linear CO₂ structure, the combination of adjacent TM atoms and Fe₆ induces bending and activation of CO₂ at the Ni site, enhancing its protonation to form key *COOH intermediate while maintaining efficient *CO desorption. The newly designed hybrid electrocatalyst demonstrates a synergistic effect of multi-metal sites in boosting CO₂ reduction to CO. Specifically, the TM atom facilitates C–Ni bond formation between the Ni site and *CO₂/*COOH species, while Fe₆ forms an Fe…O coordination bond. Detailed analysis of reaction mechanisms and energetics show that Ni-N₄, co-assisted by a single TM atom and Fe₆ (especially TM = Ni, Cu, or Ag), exhibits enhanced catalytic activity for CO production with a low limiting potential of −0.5 V. This work presents an effective strategy for improving the catalytic activity of single-atom catalysts (SACs) at high metal content.

嵌入具有 M-Nx-C 构型的掺氮碳材料中的单过渡金属 (TM) 原子已成为一类很有前途的电化学二氧化碳还原 (CO2RR) 电催化剂。然而，在 TM 原子密度较高的情况下，全面了解活性位点结构和反应机理仍是一项重大挑战，但这对提高 CO2RR 性能至关重要。在这项工作中，我们利用第一性原理计算研究了 Ni-N4 位点在邻近 TM 原子和 Fe6 纳米粒子的共同协助下将 CO2 还原成 CO 的电催化性能。与之前研究的许多保持线性 CO2 结构的 Ni-N4 催化剂不同，相邻 TM 原子和 Fe6 的结合可诱导 Ni 位点上的 CO2 发生弯曲和活化，增强其质子化以形成关键的 *COOH 中间体，同时保持高效的 *CO 解吸。新设计的混合电催化剂展示了多金属位点在促进 CO2 还原成 CO 方面的协同效应。具体来说，TM 原子促进了 Ni 位点与 *CO2/*COOH 物种之间 C-Ni 键的形成，而 Fe6 则形成了 Fe...O 配位键。对反应机理和能量学的详细分析表明，Ni-N4 在单个 TM 原子和 Fe6（尤其是 TM = Ni、Cu 或 Ag）的共同辅助下，在 -0.5 V 的低极限电位下，对 CO 的生成表现出更强的催化活性。这项研究提出了一种在高金属含量条件下提高单原子催化剂催化活性的有效策略。

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引用次数: 0

Effect of TiO2 nanoparticles on the assembly of a copolymer-clay dispersion 二氧化钛纳米颗粒对共聚物-粘土分散体组装的影响

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.152

Nanocomposites based on copolymer and clay minerals are attracting increasing attention as they are appropriate for extensive applications. In this work, we present results from an experimental study on the effects of TiO₂ nanoparticles on a pluronic-F127/laponite water solution in the sol state. Differential Scanning Calorimetry (DSC), Dynamic Light Scattering (DLS) and Fourier Transform Infrared Attenuated Total Reflection Spectroscopy (FTIR-ATR) were used to characterize the systems. By DSC and DLS measurements the occurrence of micellization was first investigated. The temperature induced self-assembly was then studied by DLS identifying three relaxations associated to differently sized diffusing structures. The correlation between dynamics and bonding structure was thoroughly investigated by analyzing some specific infrared vibrational bands. In particular, the study of the characteristic absorption band of the ether groups in the dry state allowed to evaluate the amorphous/crystalline component evidencing the presence of more extended conformations in presence of the higher TiO₂. Finally, the analysis of the bending mode for the residual water provided valuable insight about structural OH groups enabling a distinction between different types of water molecules associated to the copolymer/nanoparticle systems.

基于共聚物和粘土矿物的纳米复合材料因其应用广泛而日益受到关注。在这项工作中，我们介绍了关于二氧化钛纳米粒子对溶胶状态下的pluronic-F127/皂石水溶液的影响的实验研究结果。研究采用了差示扫描量热法（DSC）、动态光散射法（DLS）和傅立叶变换红外衰减全反射光谱法（FTIR-ATR）来表征系统。首先通过 DSC 和 DLS 测量研究了胶束化的发生。然后通过 DLS 研究了温度诱导的自组装，确定了与不同大小的扩散结构相关的三种弛豫。通过分析一些特定的红外振动波段，对动力学和键合结构之间的相关性进行了深入研究。特别是对干燥状态下醚基团的特征吸收带的研究，可以评估非晶/晶体成分，证明在较高的二氧化钛存在时，存在更多的扩展构象。最后，通过分析残留水的弯曲模式，可以深入了解羟基的结构，从而区分与共聚物/纳米粒子系统相关的不同类型的水分子。

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引用次数: 0

The influence of P-toluenesulfonyl isocyanate on the solvation structure and solid electrolyte interphase formation on graphite anode under high temperatures. 高温下对甲苯磺酸异氰酸酯对石墨阳极溶解结构和固体电解质相间形成的影响

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.153

Qianqian Wang, Ninggui Ma, Yaqin Zhang, Yu Xiong, Deshuai Yang, Pu Zhang, Jun Fan

The formation and stability of the solid electrolyte interphase (SEI) play a crucial role in determining the performance and lifespan of lithium-ion batteries (LIBs) at evaluated temperatures. Electrolyte additives have emerged as promising candidates for modulating the formation kinetics and stability of the SEI layer. In this study, molecular dynamics (MD) and ab initio molecular dynamics (AIMD) simulations were employed to investigate the influences of P-toluenesulfonyl isocyanate (PTSI) as an electrolyte additive in the LiPF₆/EC/DMC electrolyte on the SEI formation process on the graphite anode under high temperatures. MD simulations revealed that PTSI induces modifications in the solvation structure, resulting in two ethylene carbonate (EC) and two dimethyl carbonate (DMC) molecules in the first solvation shell of Li⁺. Furthermore, the PTSI additive suppressed the decomposition of solvent molecules and PF6 anions in the LiPF₆/EC/DMC/PTSI electrolyte under high temperatures according to the AIMD simulations, contributing to a more stable SEI layer. Moreover, this suppression can be attributed to the reduced reactivity of solvent molecules and salt anions, as evidenced by the enhanced bond strength and decreased bond length. These microscopic insights provide a multi-faceted understanding of the functionality of PTSI additives, facilitating the rational design of novel additives.

固体电解质相间层（SEI）的形成和稳定性对锂离子电池（LIB）在评估温度下的性能和寿命起着至关重要的作用。电解质添加剂已成为调节 SEI 层形成动力学和稳定性的有前途的候选物质。本研究采用分子动力学（MD）和非线性分子动力学（AIMD）模拟来研究 LiPF6/EC/DMC 电解液中作为电解液添加剂的对甲苯磺酰基异氰酸酯（PTSI）对高温下石墨负极 SEI 形成过程的影响。MD 模拟显示，PTSI 引发了溶解结构的改变，导致 Li+ 的第一个溶解壳中出现了两个碳酸乙烯（EC）分子和两个碳酸二甲酯（DMC）分子。此外，根据 AIMD 模拟，在高温条件下，PTSI 添加剂抑制了 LiPF6/EC/DMC/PTSI 电解液中溶剂分子和 PF6 阴离子的分解，有助于形成更稳定的 SEI 层。此外，这种抑制作用可归因于溶剂分子和盐阴离子反应性的降低，这一点可从键强度的增强和键长的降低得到证明。这些微观见解提供了对 PTSI 添加剂功能的多方面理解，有助于新型添加剂的合理设计。

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引用次数: 0

Exploring 1T/2H MoS2 quantum dots modified 2D CoPx nanosheets for efficient electrocatalytic hydrogen evolution reaction 探索 1T/2H MoS2 量子点修饰的二维 CoPx 纳米片用于高效电催化氢气进化反应。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.150

The exploration of multiphases and 0D/2D heterojunction in transition metal phosphides (TMPs) and transition metal sulfides (TMDs) is of major interest for hydrogen evolution reaction (HER). Herein, a novel combination route where 0D mixed-phased 1T/2H molybdenum sulfide quantum dots (MoS₂ QDs) are uniformly anchored on the 2D CoP_x nanosheets is developed. MoS₂ QDs and CoP_x were prepared via hydrothermal method and mixed with different ratios (Mo:Co ratios of 2:1, 1:1, and 1:2) and annealed under different temperatures to modulate their application in acidic HER processes. Specifically, 2Mo/1Co exhibited advanced performance for HER in 0.5 M H₂SO₄ solution and required 14 mV to deliver 10 mA cm⁻² and revealed a descended Tafel slope of 75.42 mV dec⁻¹ with 240 h stability except obvious deactivation. The successful design and construction of 0D/2D mixed-dimensional materials would broaden the application of MoS₂ and CoP_x for electrocatalytic hydrogen evolution.

过渡金属磷化物（TMPs）和过渡金属硫化物（TMDs）中的多相和 0D/2D 异质结的探索对于氢进化反应（HER）具有重大意义。在这里，我们开发了一种新颖的组合路线，即在二维 CoPx 纳米片上均匀锚定 0D 混合相 1T/2H 硫化钼量子点（MoS2 QDs）。MoS2 QDs 和 CoPx 通过水热法制备，并以不同比例（Mo:Co 比例为 2:1、1:1 和 1:2）混合，在不同温度下退火，以调节其在酸性 HER 过程中的应用。具体而言，2Mo/1Co 在 0.5 M H2SO4 溶液中表现出先进的 HER 性能，需要 14 mV 才能提供 10 mA cm-2，并且显示出 75.42 mV dec-1 的下降 Tafel 斜坡，除明显失活外，240 h 内保持稳定。0D/2D 混合维材料的成功设计和构建将拓宽 MoS2 和 CoPx 在电催化氢进化方面的应用。

引用次数: 0

The interstitial Ru dopant induces abundant Ni(Fe)Ru cooperative sites to promote ampere-level current density for overall water splitting 间隙掺杂的 Ru 可诱导丰富的 Ni(Fe)Ru 合作位点，从而提高安培级电流密度，实现整体水分离

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.140

Directionally induced interstitial Ru dopant rather than ordinary substitutional doping is a challenge. Furthermore, DFT calculations revealed that compared with the substituted Ru dopants, the interstitial Ru dopants induce abundant Ni(Fe)Ru cooperative sites, greatly expediting the reaction kinetics for HER and OER. Inspired by these, the interstitial Ru-doped NiFeP/NF electrode is constructed by the ’quenching doped Ru-phosphorization’ strategy. Relevant physical characterizations confirmed that interstitial Ru dopants promote electron reset in the Ni(Fe)Ru synergistic sites, effectively avoiding metal atom dissolution and encouraging more Ni (Fe)OOH active species. As expected, the Ru-NiFeP/NF||Ru-NiFeP/NF electrolyzer only need as low as 1.54 V to yield a current density of 1 A cm⁻². In summary, this work innovatively constructs the phosphide electrode with ampere-level current density from the perspective of regulating the doping position of Ru. This provides a new design idea for optimizing the Ru doping strategy.

定向诱导间隙掺杂 Ru 而不是普通的取代掺杂是一项挑战。此外，DFT 计算显示，与取代型 Ru 掺杂相比，间隙型 Ru 掺杂能诱导丰富的 Ni(Fe)Ru 合作位点，从而大大加快 HER 和 OER 的反应动力学。受此启发，我们采用 "淬火掺杂 Ru-磷化 "策略构建了间隙掺杂 Ru 的 NiFeP/NF 电极。相关的物理表征证实，间隙掺杂 Ru 可促进 Ni(Fe)Ru 协同位点的电子重置，有效避免金属原子溶解，促进更多的 Ni (Fe)OOH 活性物种。正如预期的那样，Ru-NiFeP/NF||Ru-NiFeP/NF 电解槽只需要低至 1.54 V 的电压就能产生 1 A cm-2 的电流密度。总之，这项工作从调节 Ru 掺杂位置的角度出发，创新性地构建了具有安培级电流密度的磷化电极。这为优化 Ru 掺杂策略提供了新的设计思路。

引用次数: 0

Accelerated water dissociation kinetics by nickel-nickelous hydroxide epitaxial interfaces for superior alkaline hydrogen generation 通过氢氧化镍-镍外延界面加速水解离动力学，实现卓越的碱性制氢。

IF 9.4 1区化学 Q1 CHEMISTRY, PHYSICAL

Journal of Colloid and Interface Science

Pub Date : 2024-10-28 DOI: 10.1016/j.jcis.2024.10.141

The intrinsic performance of an electrocatalyst can be reinforced by constructing appropriate epitaxial interfaces, where the modulated electronic states and adsorption/desorption behaviors are conductive to enhancing electrocatalytic activity. Herein, nickel-nickelous hydroxide epitaxial interface supported on nickel foam (Ni-Ni(OH)₂/NF) with epitaxial growth of nickel nanoparticles on the surface of nickelous hydroxide nanoribbons is devised for alkaline hydrogen evolution reaction (HER). Notably, the Ni-Ni(OH)₂/NF reveals excellent electrocatalytic activity of alkaline HER (158 mV @ 100 mA cm⁻²), along with robust stability (90 % activity retention after 150 h continuous test at 200 mA cm⁻²). Theoretical simulations disclose the tuned interface electronic structure and accelerated water dissociation around the epitaxial nickel-nickelous hydroxide interface result in efficient electrochemical activity toward alkaline hydrogen evolution.

通过构建适当的外延界面可以增强电催化剂的内在性能，其中调制的电子状态和吸附/解吸行为有利于提高电催化活性。在此，我们设计了以泡沫镍（Ni-Ni(OH)2/NF）为支撑的氢氧化镍外延界面，并在氢氧化镍纳米带表面外延生长镍纳米颗粒，用于碱性氢进化反应（HER）。值得注意的是，Ni-Ni(OH)2/NF 显示出卓越的碱性氢进化反应电催化活性（158 mV @ 100 mA cm-2）和强大的稳定性（在 200 mA cm-2 下连续测试 150 小时后活性保持率为 90%）。理论模拟显示，经过调整的界面电子结构和外延镍-氢氧化镍界面周围水的加速解离，使其具有高效的碱性氢演化电化学活性。

引用次数: 0