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Natural Hydrogen: A Mini-Review Unveiling Its Potential as a Key to Sustainable Future for Energy 天然氢:揭示其作为可持续能源未来关键潜力的小型综述
Pub Date : 2025-12-09 DOI: 10.1002/ece2.70026
Yuanming Gao, Silin Liu, Rong Chen, Zongyi Li, Xuezhen Wu, Wen Ma, Yuzhuo Luo, Yanhe Wang, Xi Ding, Xiaoxin Li, Henrietta W. Langmi, Nicholas M. Musyoka, Lei Jiang, Rodolfo Christiansen, Guo-Ming Weng

As the global energy shortage challenge and transition continues, greater attention is being drawn to natural hydrogen, a clean and high-potential energy source. This review aims to provide an overview about the formation mechanism, exploration technology, research status of revolutionary natural hydrogen, as well as its key role and potential impact in achieving a sustainable future for energy. Natural hydrogen is produced primarily through serpentinization, a process in which water reacts with iron-rich ultrabasic rocks and is hypothesized to have the potential for forming gas accumulations in certain suitable regions of the world. Although natural hydrogen reserves are presently unclear, it is a promising solution to accelerate the decarbonization of energy-intensive industries. Until now, numerous studies have been conducted in many countries and regions, leading to multiple ambitious projects (currently under construction or implementation) and demonstrating the feasibility of using existing technologies for the safe exploration of natural hydrogen. With the development of natural hydrogen, it is believed that more resources will be certainly found and the remaining issues could be resolved in the future. This work could offer important insights for the development of natural hydrogen that is a key toward a sustainable future of energy.

随着全球能源短缺挑战和转型的持续,天然氢这种清洁、高潜力的能源越来越受到人们的关注。本文综述了革命性天然氢的形成机理、勘探技术、研究现状,以及它在实现能源可持续未来中的关键作用和潜在影响。天然氢主要是通过蛇纹石作用产生的,这是一种水与富含铁的超基性岩石反应的过程,据推测,在世界上某些合适的地区,它有可能形成天然气聚集。虽然目前尚不清楚天然氢储量,但它是加速能源密集型工业脱碳的一个有希望的解决方案。到目前为止,许多国家和地区已经进行了大量的研究,导致了多个雄心勃勃的项目(目前正在建设或实施),并证明了利用现有技术安全勘探天然氢气的可行性。随着天然氢气的开发,相信未来一定会发现更多的资源,遗留的问题也会得到解决。这项工作可以为开发天然氢提供重要的见解,而天然氢是实现可持续能源未来的关键。
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引用次数: 0
Cobalt-Based Catalysts for Electrochemical Water Splitting: A Review of Mechanisms, Performance, and Applications 钴基电化学水分解催化剂:机理、性能及应用综述
Pub Date : 2025-12-08 DOI: 10.1002/ece2.70025
Yuqi Chen, Kexin Du, Junru Li, Shuyan Zheng, Min Cui, Yunxiang Ma, Jingui Wang, Shuai Wang

The development of efficient, stable, and earth-abundant electrocatalysts is critical for advancing electrochemical water splitting as a sustainable hydrogen production technology. Among non-precious candidates, cobalt-based materials have garnered significant attention due to their structural versatility and tunable electronic properties. This review comprehensively examines recent progress in cobalt-based catalysts for the hydrogen and oxygen evolution reactions. We discuss key optimization strategies, including nanostructuring, heteroatom doping, and defect/interface engineering, that enhance activity and stability by increasing active site density, improving conductivity, and optimizing intermediate adsorption energetics. A particular focus is placed on the dynamic reconstruction of pre-catalysts into active (oxy)hydroxide phases under operational conditions, a crucial consideration for rational design. By integrating mechanistic insights from advanced in situ characterization and theoretical calculations, we elucidate structure-activity relationships and reaction pathways. Finally, we outline persistent challenges and future directions, emphasizing the need for standardized evaluation and the design of durable catalysts capable of operating at industrial-scale current densities to bridge the gap between laboratory research and practical application.

开发高效、稳定、储量丰富的电催化剂是推动电化学水分解作为一种可持续制氢技术的关键。在非珍贵的候选材料中,钴基材料由于其结构的多功能性和可调谐的电子特性而获得了极大的关注。本文综述了近年来钴基析氢、析氧催化剂的研究进展。我们讨论了关键的优化策略,包括纳米结构、杂原子掺杂和缺陷/界面工程,通过增加活性位点密度、改善电导率和优化中间吸附能量来增强活性和稳定性。特别关注预催化剂在操作条件下动态重构为活性(氧)氢氧化物相,这是合理设计的关键考虑因素。通过整合先进的原位表征和理论计算的机理见解,我们阐明了结构-活性关系和反应途径。最后,我们概述了持续的挑战和未来的方向,强调需要标准化评估和设计能够在工业规模电流密度下运行的耐用催化剂,以弥合实验室研究和实际应用之间的差距。
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引用次数: 0
Synergistic Design of MXene Architectures for Mechanically Robust and High-Performance Flexible Batteries and Supercapacitors 机械坚固和高性能柔性电池和超级电容器的MXene架构协同设计
Pub Date : 2025-11-27 DOI: 10.1002/ece2.70018
Narasimharao Kitchamsetti, Sungwook Mhin

The rapid advancement in wearable, portable, and foldable electronic devices has underscored inherent deficiencies in conventional energy storage technologies, particularly with respect to mechanical compliance and device miniaturization. Overcoming these limitations demands energy storage solutions that integrate high electrochemical performance with mechanical resilience and scalability. In this context, MXenes, two-dimensional (2D) transition metal carbides, nitrides, or carbonitrides, have emerged as promising candidates due to their outstanding electrical conductivity, tunable surface chemistry, and intrinsic flexibility. Unlike previous reviews that focus primarily on MXene synthesis or individual device performance, this work provides a synergistic and cross-disciplinary perspective on the structural design of MXene architectures for flexible energy storage systems. It critically correlates hierarchical structural engineering (such as composite integration, dimensional hybridization, and interface modulation) with the mechanical and electrochemical behaviors of MXenes in various device configurations, including flexible batteries and supercapacitors (SCs). Particular attention is given to mechanical-electrochemical coupling mechanisms that govern flexibility retention, strain accommodation, and charge transport dynamics. Furthermore, this review offers a comparative discussion across multiple chemistries, encompassing Li-, Na-, Zn-, and K-ion batteries and SCs, thereby providing an integrative understanding of MXene functionality beyond single-system studies. Finally, this review outlines emerging design principles, fabrication strategies, and research directions aimed at achieving scalable, durable, and high-performance MXene-based flexible energy storage technologies. This synergistic perspective bridges the gap between mechanical engineering and electrochemical optimization, offering new insights for the next generation of flexible and wearable power systems.

可穿戴、便携式和可折叠电子设备的快速发展凸显了传统储能技术固有的缺陷,特别是在机械顺应性和设备小型化方面。克服这些限制需要将高电化学性能与机械弹性和可扩展性相结合的储能解决方案。在这种情况下,MXenes,二维(2D)过渡金属碳化物,氮化物或碳氮化物,由于其出色的导电性,可调谐的表面化学性质和固有的灵活性而成为有希望的候选者。与之前主要关注MXene合成或单个器件性能的综述不同,这项工作为灵活储能系统的MXene架构的结构设计提供了协同和跨学科的视角。它将分层结构工程(如复合集成、尺寸杂交和界面调制)与MXenes在各种设备配置(包括柔性电池和超级电容器(SCs))中的机械和电化学行为密切相关。特别关注机械-电化学耦合机制,控制柔韧性保持,应变调节和电荷传输动力学。此外,本综述提供了多种化学物质的比较讨论,包括Li-、Na-、Zn-、k -离子电池和sc,从而提供了对MXene功能的综合理解,超越了单一系统的研究。最后,本文概述了新兴的设计原则、制造策略和研究方向,旨在实现可扩展、耐用和高性能的基于mxene的柔性储能技术。这种协同的观点弥合了机械工程和电化学优化之间的差距,为下一代灵活和可穿戴的电力系统提供了新的见解。
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引用次数: 0
Exceptionally Durable CO2 Photoreduction Mediated by Defect-Engineered CaIn2S4 Nanoflowers 缺陷工程CaIn2S4纳米花介导的异常持久的CO2光还原
Pub Date : 2025-11-23 DOI: 10.1002/ece2.70020
Jiaming Li, Yihui Du, Kai Wang

Solar-driven CO2 reduction faces major limitations due to insufficient photoabsorption, delayed electron-hole separation, and a significant CO2 activation barrier. Defect engineering was used to optimize these vital processes. As a prototype, typical nontoxic ternary sulfide CaIn2S4 (CIS) nanoflowers were designed, and abundant sulfur vacancies were deliberately created on their surfaces. The charge delocalization around the sulfur vacancies contributes to CO2 conversion into the *COOH intermediate, which was confirmed by in situ Fourier-transform infrared spectroscopy. Ultrafast transient absorption spectroscopy manifests the sulfur vacancy that allows for a ∼1.3-fold increase in average recovery lifetime, confirmed by photoelectrochemical analysis and DFT calculations, which ensure promoted carrier separation rates. Consequently, the CISv demonstrates a CO rate of 10.95 μmol g−1 h−1, which is about 6.5 times greater than the pristine CIS nanoflowers, and its photocatalytic activity remains almost unchanged after 120 h of photocatalysis. Our findings will stimulate further research on vacancy-containing catalyst design for CO2 reduction to hydrocarbons.

由于光吸收不足、电子空穴分离延迟以及显著的CO2激活屏障,太阳能驱动的CO2减排面临主要限制。缺陷工程被用来优化这些重要的过程。设计了典型的无毒三元硫化物CaIn2S4 (CIS)纳米花,并在其表面故意制造了丰富的硫空位。硫空位周围的电荷离域有助于CO2转化为*COOH中间体,这一点通过原位傅里叶变换红外光谱得到了证实。超快瞬态吸收光谱显示,硫空位允许平均回收寿命增加~ 1.3倍,由光电化学分析和DFT计算证实,这确保了促进载流子分离率。结果表明,CISv纳米花的CO速率为10.95 μmol g−1 h−1,是原始CIS纳米花的6.5倍,并且在光催化120 h后其光催化活性基本保持不变。我们的发现将激发对含空催化剂设计的进一步研究,以将二氧化碳还原为碳氢化合物。
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引用次数: 0
Layered Perovskite Materials for Photocatalytic Overall Water Splitting: Recent Advances, Enhanced Strategies, and Future Challenges 层状钙钛矿材料用于光催化整体水分解:最新进展,增强策略和未来挑战
Pub Date : 2025-11-23 DOI: 10.1002/ece2.70023
Na Li, Chao Cheng, Yilin Wang, Alex W. Robertson, Zhenyu Sun

Achieving sustainable energy generation without causing environmental pollution is one of modern society's grand challenges. Photocatalytic overall water splitting (OWS) presents a sustainable option for producing the green energy vector H2 while eliminating the need for sacrificial agents. However, the selection of appropriate catalysts is essential for the practical viability of this approach. Among various photocatalytic materials, layered perovskites have attracted significant attention due to their compositional flexibility and attractive hybrid electronic band structure. Moreover, their intrinsic layered architecture promotes charge separation, which further enhances photocatalytic performance. Therefore, layered perovskites are considered promising candidates for photocatalytic OWS. Herein, this review classifies and summarizes the research progress of (100)-, (110)-, and (111)-type layered perovskite photocatalysts for OWS. We first introduce the basic principle of photocatalytic OWS, followed by a discussion of the advantages and challenges of employing layered perovskites as OWS photocatalysts. The relevant properties of layered perovskite photocatalysts that influence OWS performance are analyzed. Furthermore, experimental strategies such as doping, composite structure construction, and morphology modulation are comprehensively reviewed to highlight their roles in enhancing photocatalytic efficiency. Finally, current limitations and future research directions for layered perovskite-based OWS are outlined to guide further developments in this field.

在不造成环境污染的情况下实现可持续能源生产是现代社会面临的重大挑战之一。光催化全面水分解(OWS)为生产绿色能源载体H2提供了一种可持续的选择,同时消除了对牺牲剂的需求。然而,选择合适的催化剂对于这种方法的实际可行性至关重要。在各种光催化材料中,层状钙钛矿由于其组成的灵活性和具有吸引力的杂化电子带结构而备受关注。此外,它们固有的层状结构促进了电荷分离,从而进一步提高了光催化性能。因此,层状钙钛矿被认为是光催化OWS的有希望的候选者。本文对OWS用(100)-、(110)-和(111)型层状钙钛矿光催化剂的研究进展进行了分类和总结。我们首先介绍了光催化OWS的基本原理,然后讨论了使用层状钙钛矿作为OWS光催化剂的优点和挑战。分析了层状钙钛矿光催化剂的相关性质对OWS性能的影响。此外,本文还对掺杂、复合材料结构构建和形态调制等实验策略进行了综述,重点介绍了它们在提高光催化效率方面的作用。最后,概述了层状钙钛矿OWS目前的局限性和未来的研究方向,以指导该领域的进一步发展。
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引用次数: 0
Temperature Self-Regulation, Energy Storage, and Fire Safety Intelligent Wood for Safe and Energy-Efficient Buildings 面向安全节能建筑的温度自我调节、储能和消防安全智能木材
Pub Date : 2025-11-20 DOI: 10.1002/ece2.70019
Kai Xu, Mixue Li, Ao Qin, Chentao Yan, Yue Xu, Shuhui Liang, Bin Li, Serge Bourbigot, Lubin Liu

With the intensification of the global energy and environmental crises, organic phase change energy storage materials (OPCM) are widely used in energy efficient buildings. However, conventional OPCM are easily flammable and prone to leak, which restricts their applications in emerging fields. Herein, a novel intrinsic flame retardant OPCM (bis (polyethylene glycol) methyl phosphonate, BPMP) was successfully synthesized by the nucleophilic substitution reaction of polyethylene glycol (PEG) and methyl phosphorus dichloride. Compared with conventional OPCM, BPMP is almost incapable of being ignited and maintains a phase change latent heat (153.57 J/g) similar to that of PEG. Subsequently, flame-retardant energy-storage transparent wood (FOPTW) was prepared by vacuum pressure impregnation of BPMP into the delignified cellulose frame. Due to the capillary action and intermolecular hydrogen bonding of wood stencil, FOPTW exhibited excellent leak resistance and reinforcement properties. The enthalpy of FOPTW was up to 77.23 J/g with only minor changes after 50 cycles. Meanwhile, FOPTW can realize the immediate extinguishment effect from fire, and its rate and total amount of heat release are 17% and 50.7% lower than those of OPTW. It is attributed to the gas-phase radical trapping and condensed-phase catalytic charring effect of BPMP in FOPTW. Meanwhile, the phase transition latent heat process of FOPTW is used to embed temperature sensors inside it and construct thermal runaway warning devices, thus realizing active and repetitive high temperature warnings for OPCM. This bio-based energy storage material with multiple fire safety protection systems provides a novel design idea for creating intelligent, green, and safe buildings in the 21st century.

随着全球能源和环境危机的加剧,有机相变储能材料(OPCM)在节能建筑中得到了广泛的应用。然而,传统的OPCM容易易燃,容易泄漏,这限制了它们在新兴领域的应用。本文通过聚乙二醇(PEG)与二氯化甲基磷的亲核取代反应,成功合成了一种新型特性阻燃剂OPCM(双聚乙二醇甲基膦酸酯,BPMP)。与常规OPCM相比,BPMP几乎不能被点燃,并保持与PEG相似的相变潜热(153.57 J/g)。随后,将BPMP真空加压浸渍到脱木质素纤维素框架中,制备了阻燃储能透明木(FOPTW)。由于木模板的毛细作用和分子间氢键作用,FOPTW具有优异的防漏和增强性能。循环50次后,FOPTW的焓值达到77.23 J/g,变化不大。同时,FOPTW可以实现火源的即时灭火效果,其放热速率和放热总量比OPTW低17%和50.7%。这归因于BPMP在FOPTW中的气相自由基捕获和冷凝相催化炭化作用。同时,利用FOPTW的相变潜热过程,在其内部嵌入温度传感器,构建热失控预警装置,实现对OPCM的主动重复高温预警。这种具有多种消防安全防护系统的生物基储能材料,为创造21世纪智能、绿色、安全的建筑提供了一种新颖的设计思路。
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引用次数: 0
Engineering Electrocatalytic Structures Through Molten Salt-Mediated Mechanistic Control 熔盐介导的工程电催化结构机理控制
Pub Date : 2025-11-20 DOI: 10.1002/ece2.70022
Yutong Feng, Mingjie Wang, Hanyuan Zhang, Shutong Qin, Tianqi Guan, Bohao Chang, Weilin Xu, Yujie Ma, Jun Wan

Molten salt synthesis has emerged as a versatile platform for the structural engineering of electrocatalysts, offering distinct advantages in controlling phase composition, morphology, and defect chemistry under thermodynamically and kinetically favorable conditions. However, critical challenges remain in elucidating the underlying mechanisms of molten salt-mediated transformations, particularly regarding the influence of salt composition, redox activity, and thermal behavior on structural evolution and catalytic properties. This review provides a materials-centered analysis of molten salt synthesis, emphasizing its structural modulation capabilities relative to conventional approaches. It systematically discusses six major classes of electrocatalysts: carbon-based materials, metals and alloys, metal oxides, metal carbides and nitrides, metal sulfides and phosphides, and hybrid composites. The unique advantages of molten salt environments are highlighted in enabling controlled nanoscale architecture, tunable porosity, precise crystallographic orientation, and effective surface/interface engineering. These features facilitate the formation of metastable phases, high-index facets, hierarchical porosity, and active defect sites, collectively enhancing charge transfer, active site exposure, and durability of catalysts. By correlating molten salt-induced structural features with improved performance in water splitting, oxygen reduction, and carbon dioxide reduction, this review establishes a unified framework for catalyst design and offers mechanistic insights to guide future development of high-efficiency electrocatalysts via molten salt strategies.

熔盐合成已成为电催化剂结构工程的通用平台,在热力学和动力学有利条件下,在控制相组成、形貌和缺陷化学方面具有明显的优势。然而,在阐明熔盐介导转化的潜在机制方面,特别是在盐成分、氧化还原活性和热行为对结构演变和催化性能的影响方面,仍然存在重大挑战。这篇综述提供了以材料为中心的熔盐合成分析,强调其相对于传统方法的结构调制能力。它系统地讨论了六大类电催化剂:碳基材料、金属和合金、金属氧化物、金属碳化物和氮化物、金属硫化物和磷化物以及杂化复合材料。熔盐环境的独特优势在实现可控的纳米级结构、可调的孔隙度、精确的晶体取向和有效的表面/界面工程方面得到了强调。这些特征促进了亚稳相、高指数面、分层孔隙和活性缺陷位点的形成,共同增强了催化剂的电荷转移、活性位点暴露和耐久性。通过将熔盐诱导的结构特征与水分解、氧还原和二氧化碳还原性能的改善联系起来,本文建立了一个统一的催化剂设计框架,并为通过熔盐策略指导未来高效电催化剂的开发提供了机制见解。
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引用次数: 0
Thermal Shock Induced Oxygen Vacancies-Rich TiO2 Supported Pt Nanoparticles for Boosting Hydrogen Evolution Reaction 热冲击诱导富氧空位的TiO2负载Pt纳米颗粒促进析氢反应
Pub Date : 2025-11-19 DOI: 10.1002/ece2.70021
Jinzheng Liu, Junwei Sun, Xiaoxia Wang, Yue Wang, Meiyue Li, Mingzhu Li, Xiaoyan Zhang, Hongyin Xia, Jiankun Sun, Daohao Li, Lixue Zhang

The regulation of oxygen vacancies in metal oxide matrices is crucial for achieving efficient supported catalysts, albeit posing significant challenges. In this work, we propose a facile thermal shock method as an alternative to the conventional prolonged calcination process for synthesizing highly dispersed Pt nanoparticles supported on a TiO2 substrate with abundant oxygen vacancies (referred to as Pt@Ov-TiO2), which is achieved by utilizing a movable hot bed that shuttled between a high temperature heating zone and a liquid nitrogen cooling zone. A sudden heating-to-cooling pyrolytic conversion process spanning not only endows substrates with abundant oxygen vacancies but also yields small and well-dispersed noble metal nanoparticles. The Pt@Ov–TiO2 catalyst demonstrates exceptional electrocatalytic hydrogen evolution reaction (HER) performance in acidic media, achieving a current density of 10 mA cm−2 at a low potential of 39.9 mV. Furthermore, it exhibits superior mass activity and remarkable stability compared to commercial Pt/C catalysts. Density functional theory (DFT) calculations demonstrate the introduction of oxygen vacancies contributes to a stronger interaction between TiO2 substrate and Pt, optimizing the free energy of hydrogen adsorption on the electron-rich Pt species, thereby enhancing the electrocatalytic HER performance. This finding provides a pathway for understanding the synergistic modulation of support defects and noble metal particles, thereby optimizing the interaction between the support and metal in substrate-supported metal electrocatalysts for highly efficient hydrogen production.

金属氧化物基质中氧空位的调节对于实现高效负载催化剂至关重要,尽管存在重大挑战。在这项工作中,我们提出了一种简单的热冲击方法,作为传统的长时间煅烧过程的替代方法,用于合成高度分散的Pt纳米颗粒,支撑在具有丰富氧空位的TiO2衬底上(称为Pt@Ov-TiO2),这是通过利用在高温加热区和液氮冷却区之间穿梭的可移动热床来实现的。突然加热到冷却的热解转化过程不仅赋予了衬底丰富的氧空位,而且产生了小而分散良好的贵金属纳米颗粒。Pt@Ov -TiO2催化剂在酸性介质中表现出优异的电催化析氢反应(HER)性能,在39.9 mV的低电位下达到10 mA cm−2的电流密度。此外,与商业Pt/C催化剂相比,它具有优越的质量活性和显著的稳定性。密度泛函理论(DFT)计算表明,氧空位的引入有助于TiO2衬底与Pt之间更强的相互作用,优化氢在富电子Pt上的吸附自由能,从而提高电催化HER性能。这一发现为理解载体缺陷和贵金属颗粒的协同调节提供了一条途径,从而优化了载体和金属在底物负载金属电催化剂中的相互作用,以实现高效制氢。
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引用次数: 0
Low-Content Co-Modified Carbon Nitride With Co-N Bond as an Efficient and Stable Catalyst for Electrocatalytic Oxidation of 5-Hydroxymethylfurfural 含Co-N键的低含量共改性氮化碳电催化氧化5-羟甲基糠醛的高效稳定催化剂
Pub Date : 2025-11-19 DOI: 10.1002/ece2.70024
Hao Feng, Liying Fu, Jianfei Li, Xuxia Chen, Lina Wu, Terence Xiaoteng Liu, Guangbo Che, Yonghui Gao, Chunbo Liu

The traditional noble metal and transition metal catalysts encounter challenges due to the high cost and potential environmental pollution in the electrocatalytic 5-hydroxymethylfurfural oxidation reaction (HMFOR). The construction of the Co-N bond not only can reduce the excessive use of metals but also effectively enhances the electrocatalytic performance by increasing the electron transfer rate and promoting the adsorption of key intermediates. In this work, low-content Co-modified carbon nitride (CN) with a Co-N bond (1% Co-CN/NF) was constructed as an electrocatalytic catalyst for HMFOR, and excellent FDCA production yield could be achieved in both low-concentration (10 mM) and high-concentration HMF (100 mM). In situ/ex situ characterization combined with DFT calculation confirmed that the formation of the Co-N bond enhanced the electron transport rate during the HMFOR process, reduced the adsorption potential of HMF on the electrode, and promoted the adsorption of HMF; thus, the HMFOR performance was effectively improved. Subsequently, based on its potential application prospects, the experimental conditions were optimized by the XGBoost model of machine learning (ML) to achieve obvious performance improvement (achieving 100% of HMF conversion, 99.04% of FDCA yield, 98.86% of FE, and 24 cycles of stability) in 10 mM HMF, and the results were higher than those of currently reported organic electrocatalysts and even most Co-based electrocatalysts. It was exciting that superior FDCA productivity yield and recovery yield were obtained in a photovoltaic electrocatalysis (PVEC) system with 100 mM HMF. This work is expected to provide precise and detailed insights into the further construction of a novel low-budget, environmentally friendly, efficient, and stable HMFOR system.

在电催化5-羟甲基糠醛氧化反应(HMFOR)中,传统的贵金属和过渡金属催化剂由于成本高和潜在的环境污染而面临挑战。Co-N键的构建不仅可以减少金属的过量使用,还可以通过提高电子转移速率和促进关键中间体的吸附,有效地提高电催化性能。本研究构建了含Co-N键的低含量共改性氮化碳(CN) (1% Co-CN/NF)作为HMFOR的电催化催化剂,在低浓度(10 mM)和高浓度HMF (100 mM)条件下均可获得优异的FDCA产率。原位/非原位表征结合DFT计算证实,Co-N键的形成增强了HMFOR过程中的电子传递速率,降低了HMF在电极上的吸附势,促进了HMF的吸附;从而有效地提高了HMFOR的性能。随后,基于其潜在的应用前景,通过机器学习(ML)的XGBoost模型对实验条件进行优化,在10 mM的HMF中实现了明显的性能提升(HMF转化率达到100%,FDCA收率达到99.04%,FE收率达到98.86%,稳定性达到24次循环),并且结果高于目前报道的有机电催化剂,甚至大多数co基电催化剂。令人兴奋的是,在100 mM HMF的光伏电催化(PVEC)系统中获得了优异的FDCA产率和回收率。这项工作有望为进一步构建新型低预算、环保、高效和稳定的HMFOR系统提供精确和详细的见解。
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引用次数: 0
Biological Zwitterion Betaine-Assisted Wide Voltage Window and Freeze-Resistance Hydrogel Electrolyte for Flexible Supercapacitor 生物两性离子甜菜碱辅助柔性超级电容器的宽电压窗和抗冻水凝胶电解质
Pub Date : 2025-11-07 DOI: 10.1002/ece2.70017
Ben Xu, Xuehao Bi, Yuxin Chen, Qun Ma, Binggang Li, Yutong Wang, Jiliu Li, Jiale Li, Ye Li, Fangna Dai

Flexible supercapacitors based on hydrogels have developed rapidly, although they still face issues such as low voltage window and easy freezing of gel at low temperatures. Herein, the biological zwitterionic betaine is utilized to lock water molecular for widening the voltage window and improving anti-freezing performances of PAM/PEG/CS/Betaine-composited hydrogels (named as PPCBx, x denotes the amount of betaine). By optimizing the betaine contents, the PPCB0.03 hydrogel reaches the stress limit of 102.04 KPa at the tensile strain limit of 400%, with a high ionic conductivity of 2.87 S m−1. The ionic conductivity remains at 0.45 and 0.15 S m−1 even at −30 and −50°C. The assembled supercapacitor can endow a high voltage window reaching 2.4 V. The specific area capacity of the device is 585.45 mF cm−2 at the current density of 2 mA cm−2 and maintains 82% after 9000 cycles. The specific capacity can still remain 191.24 mF cm−2 even at −50°C, demonstrating its remarkable anti-freezing feature. Assembled with solar cells, the device can be successfully utilized for energy harvesting.

基于水凝胶的柔性超级电容器发展迅速,但仍面临电压窗低、凝胶在低温下易冻结等问题。本文利用生物两性离子甜菜碱锁住水分子,扩大了PAM/PEG/CS/甜菜碱复合水凝胶(命名为PPCBx, x为甜菜碱用量)的电压窗,提高了其抗冻性能。通过优化甜菜碱含量,PPCB0.03水凝胶在拉伸应变极限为400%时达到102.04 KPa的应力极限,离子电导率高达2.87 S m−1。在−30和−50℃时,离子电导率分别保持在0.45和0.15 S m−1。组装好的超级电容器可以提供2.4 V的高电压窗口。在电流密度为2ma cm−2时,器件的比面积容量为585.45 mF cm−2,在9000次循环后保持82%。在- 50°C时,其比容量仍可保持191.24 mF cm−2,具有显著的防冻性能。该装置与太阳能电池组装在一起,可以成功地用于能量收集。
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