Berhanu Telay Mekonnen, Guan-Cheng Chen, Sun-Tang Chang, Yao-Ming Wang, Sheng-Yu Wang and Chen-Hao Wang
This study describes the synthesis of high-performance cauliflower-like NiMoP nanosphere electrocatalysts on a titanium mesh via a scalable pulse electrodeposition technique. The optimized cauliflower-like NiMoP demonstrates remarkable activity for the hydrogen evolution reaction in alkaline seawater, requiring only 50.3 mV overpotential to drive 10 mA cm−2 and exhibiting exceptional durability, with only 0.5% current degradation over 24 hours. This superior performance is attributed to a unique combination of an amorphous structure, a high-surface-area morphology, and synergistic electronic effects among the Ni, Mo, and P components. This work not only presents a top-tier catalyst but also validates pulse electrodeposition as a powerful strategy for engineering catalyst architecture and electronic properties, opening a promising pathway for scalable and efficient hydrogen generation directly from saline environments.
本研究描述了利用可扩展脉冲电沉积技术在钛网上合成高性能花椰菜状NiMoP纳米球电催化剂。优化后的菜花状NiMoP在碱性海水中表现出显著的析氢活性,仅需50.3 mV过电位即可驱动10 mA cm - 2,并且具有优异的耐久性,24小时内电流降解率仅为0.5%。这种优异的性能归功于非晶结构、高表面积形态和Ni、Mo和P组分之间的协同电子效应的独特组合。这项工作不仅展示了一种顶级催化剂,而且验证了脉冲电沉积作为一种强大的工程催化剂结构和电子性能策略,为直接从盐水环境中可扩展和高效地制氢开辟了一条有前途的途径。
{"title":"Highly durable and efficient hydrogen production from alkaline seawater using pulse-deposited NiMoP nanosphere electrocatalysts","authors":"Berhanu Telay Mekonnen, Guan-Cheng Chen, Sun-Tang Chang, Yao-Ming Wang, Sheng-Yu Wang and Chen-Hao Wang","doi":"10.1039/D5SE01340B","DOIUrl":"https://doi.org/10.1039/D5SE01340B","url":null,"abstract":"<p >This study describes the synthesis of high-performance cauliflower-like NiMoP nanosphere electrocatalysts on a titanium mesh <em>via</em> a scalable pulse electrodeposition technique. The optimized cauliflower-like NiMoP demonstrates remarkable activity for the hydrogen evolution reaction in alkaline seawater, requiring only 50.3 mV overpotential to drive 10 mA cm<small><sup>−2</sup></small> and exhibiting exceptional durability, with only 0.5% current degradation over 24 hours. This superior performance is attributed to a unique combination of an amorphous structure, a high-surface-area morphology, and synergistic electronic effects among the Ni, Mo, and P components. This work not only presents a top-tier catalyst but also validates pulse electrodeposition as a powerful strategy for engineering catalyst architecture and electronic properties, opening a promising pathway for scalable and efficient hydrogen generation directly from saline environments.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6811-6821"},"PeriodicalIF":4.1,"publicationDate":"2025-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yongfeng Yan, Chuanjun Xu, Ziming Zhou, Haopeng Ren, Jingjun Lin and Lipeng He
In this paper, we propose a magnet-assisted chaotic pendulum low-frequency piezoelectric energy harvester (MCP-PEH) for wave energy, designed to supply power to ocean wireless sensing equipment. The chaotic pendulum consists of a double pendulum. The main pendulum converts external excitation into internal mechanical swing, while the internal pendulum uses a rotating multistage mass to achieve frequency conversion. This design enables a better output response in the low-frequency ocean environment. The magnet-assisted mechanism allows the harvester to achieve an effective output at 0.4 Hz, reducing the starting frequency and achieving low-frequency broadband performance. Additionally, the electrical signal generated by the bottom piezoelectric sheet can be used to monitor the wave frequency. Theoretical analysis and prototype experiments are conducted to identify the main variables affecting the device, thereby proving its feasibility. Under the optimal load, the magnet-assisted mechanism increases the overall output power by 46.7%, enabling the device to generate 6.57 mW of power. Water tank experiments and energy supply analysis of the sensor further demonstrate the device's practicality and feasibility for powering ocean wireless sensing equipment.
{"title":"A magnet-assisted chaotic pendulum low-frequency piezoelectric energy harvester","authors":"Yongfeng Yan, Chuanjun Xu, Ziming Zhou, Haopeng Ren, Jingjun Lin and Lipeng He","doi":"10.1039/D5SE01119A","DOIUrl":"https://doi.org/10.1039/D5SE01119A","url":null,"abstract":"<p >In this paper, we propose a magnet-assisted chaotic pendulum low-frequency piezoelectric energy harvester (MCP-PEH) for wave energy, designed to supply power to ocean wireless sensing equipment. The chaotic pendulum consists of a double pendulum. The main pendulum converts external excitation into internal mechanical swing, while the internal pendulum uses a rotating multistage mass to achieve frequency conversion. This design enables a better output response in the low-frequency ocean environment. The magnet-assisted mechanism allows the harvester to achieve an effective output at 0.4 Hz, reducing the starting frequency and achieving low-frequency broadband performance. Additionally, the electrical signal generated by the bottom piezoelectric sheet can be used to monitor the wave frequency. Theoretical analysis and prototype experiments are conducted to identify the main variables affecting the device, thereby proving its feasibility. Under the optimal load, the magnet-assisted mechanism increases the overall output power by 46.7%, enabling the device to generate 6.57 mW of power. Water tank experiments and energy supply analysis of the sensor further demonstrate the device's practicality and feasibility for powering ocean wireless sensing equipment.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6695-6713"},"PeriodicalIF":4.1,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anaerobic fungi, primarily found in the digestive tracts of herbivores, possess remarkable capabilities to degrade lignocellulosic biomass, positioning them as pivotal contributors to sustainable biofuel production. This review explores the enzymatic arsenal of these fungi, which includes cellulases, hemicellulases, and cellulosomes comprising glycoside hydrolases (GHs), carbohydrate esterases (CEs), polysaccharide lyases (PLs), and carbohydrate-binding modules (CBMs), emphasizing their superior efficiency in breaking down recalcitrant plant materials compared to other microorganisms. We highlight their potential in bioenergy applications, such as enhancing biomethane production through synergistic interactions with methanogens. Furthermore, the review underscores the unique characteristics of anaerobic fungi, including hydrogenosome-driven metabolism, their adaptation to diverse anaerobic environments, and their role in reducing the environmental impact of biofuel production. While challenges in cultivation, genetic engineering, and large-scale application persist, advancing research into these microorganisms could unlock innovative solutions for lignocellulosic biomass utilization, paving the way for a greener energy future. This review sheds light on their untapped biotechnological potential and offers a roadmap for addressing existing barriers to their application.
{"title":"From gut to green energy: the essential role of anaerobic fungi in sustainable biofuel production","authors":"Payal Deshpande and Prashant K. Dhakephalkar","doi":"10.1039/D5SE00240K","DOIUrl":"https://doi.org/10.1039/D5SE00240K","url":null,"abstract":"<p >Anaerobic fungi, primarily found in the digestive tracts of herbivores, possess remarkable capabilities to degrade lignocellulosic biomass, positioning them as pivotal contributors to sustainable biofuel production. This review explores the enzymatic arsenal of these fungi, which includes cellulases, hemicellulases, and cellulosomes comprising glycoside hydrolases (GHs), carbohydrate esterases (CEs), polysaccharide lyases (PLs), and carbohydrate-binding modules (CBMs), emphasizing their superior efficiency in breaking down recalcitrant plant materials compared to other microorganisms. We highlight their potential in bioenergy applications, such as enhancing biomethane production through synergistic interactions with methanogens. Furthermore, the review underscores the unique characteristics of anaerobic fungi, including hydrogenosome-driven metabolism, their adaptation to diverse anaerobic environments, and their role in reducing the environmental impact of biofuel production. While challenges in cultivation, genetic engineering, and large-scale application persist, advancing research into these microorganisms could unlock innovative solutions for lignocellulosic biomass utilization, paving the way for a greener energy future. This review sheds light on their untapped biotechnological potential and offers a roadmap for addressing existing barriers to their application.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6642-6664"},"PeriodicalIF":4.1,"publicationDate":"2025-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The ocean contains a vast source of energy, and triboelectric nanogenerators (TENGs) are emerging as a promising technology for its harvesting. Here, we report a facile-fabricated, robust hybrid TENG (H-TENG) designed to simultaneously harvest wind and water flow energy. The device, fabricated using 3D and electronic design automation (EDA) technologies, comprises an upper wind-driven unit (WH-TENG) and a lower water flow-driven unit (WFH-TENG). WH-TENG utilizes rabbit fur to achieve a high short-circuit current (Isc) of 14.8 µA and a peak power of 3.54 mW, demonstrating exceptional durability by retaining 92% of its initial charge transfer (130.9 nC) after seven weeks. WFH-TENG, designed for simple preparation and integration, delivers a peak power of 1.13 mW. As a practical application, the integrated H-TENG successfully powers a water level alarm within 150 s. This work demonstrates a viable strategy for multi-energy harvesting in marine environments, paving the way for the long-term and comprehensive utilization of ocean energy.
{"title":"Facile and robust hybrid TENG for harvesting wind energy and water flow energy","authors":"Jiaxi Hu, Mengfan Li, Ying Lou, Weiqi Cui, Jiaodi Li, Qiuxiang Wang, Aifang Yu and Junyi Zhai","doi":"10.1039/D5SE01144B","DOIUrl":"https://doi.org/10.1039/D5SE01144B","url":null,"abstract":"<p >The ocean contains a vast source of energy, and triboelectric nanogenerators (TENGs) are emerging as a promising technology for its harvesting. Here, we report a facile-fabricated, robust hybrid TENG (H-TENG) designed to simultaneously harvest wind and water flow energy. The device, fabricated using 3D and electronic design automation (EDA) technologies, comprises an upper wind-driven unit (WH-TENG) and a lower water flow-driven unit (WFH-TENG). WH-TENG utilizes rabbit fur to achieve a high short-circuit current (<em>I</em><small><sub>sc</sub></small>) of 14.8 µA and a peak power of 3.54 mW, demonstrating exceptional durability by retaining 92% of its initial charge transfer (130.9 nC) after seven weeks. WFH-TENG, designed for simple preparation and integration, delivers a peak power of 1.13 mW. As a practical application, the integrated H-TENG successfully powers a water level alarm within 150 s. This work demonstrates a viable strategy for multi-energy harvesting in marine environments, paving the way for the long-term and comprehensive utilization of ocean energy.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6853-6862"},"PeriodicalIF":4.1,"publicationDate":"2025-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se01144b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this study, a novel chemical looping ammonia cracking (CLCr) process was designed for efficient hydrogen production. A closed-loop, three-reactor chemical looping system using iron oxide as the oxygen carrier was modelled in Aspen Plus. A parametric study was carried out to evaluate the effect of key parameters, including the air reactor outlet temperature, fuel reactor outlet temperature, ammonia to oxygen carrier ratio, and the steam reactor pressure. The optimal operating conditions were then identified, under which a hydrogen yield of 69.4% with 99.99% purity can be achieved with an overall energy efficiency of 79.6%. An energy balance analysis was also carried out to confirm that the process is autothermal, and the overall exergy efficiency of the process was 70.4%. These findings highlight the novel CLCr process as an energy-efficient alternative to conventional ammonia catalytic cracking for hydrogen production.
{"title":"Process modelling and thermodynamic analysis of hydrogen production through chemical looping ammonia cracking","authors":"Anantha Krishnan Vinayak Soman, Siqi Wang, Ziqi Shen and Mingming Zhu","doi":"10.1039/D5SE01010A","DOIUrl":"https://doi.org/10.1039/D5SE01010A","url":null,"abstract":"<p >In this study, a novel chemical looping ammonia cracking (CLCr) process was designed for efficient hydrogen production. A closed-loop, three-reactor chemical looping system using iron oxide as the oxygen carrier was modelled in Aspen Plus. A parametric study was carried out to evaluate the effect of key parameters, including the air reactor outlet temperature, fuel reactor outlet temperature, ammonia to oxygen carrier ratio, and the steam reactor pressure. The optimal operating conditions were then identified, under which a hydrogen yield of 69.4% with 99.99% purity can be achieved with an overall energy efficiency of 79.6%. An energy balance analysis was also carried out to confirm that the process is autothermal, and the overall exergy efficiency of the process was 70.4%. These findings highlight the novel CLCr process as an energy-efficient alternative to conventional ammonia catalytic cracking for hydrogen production.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6761-6771"},"PeriodicalIF":4.1,"publicationDate":"2025-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se01010a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652224","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chunmei Ban, Guillermo A. Ferrero, Marta Sevilla and Feixiang Wu
A graphical abstract is available for this content
此内容的图形摘要可用
{"title":"Introduction to next-generation battery technologies beyond lithium","authors":"Chunmei Ban, Guillermo A. Ferrero, Marta Sevilla and Feixiang Wu","doi":"10.1039/D5SE90078F","DOIUrl":"https://doi.org/10.1039/D5SE90078F","url":null,"abstract":"<p >A graphical abstract is available for this content</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 23","pages":" 6323-6323"},"PeriodicalIF":4.1,"publicationDate":"2025-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145537643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Konstantin Skudler, Rukiya Matsidik, Ayda Gholamhosseinian, Hongfei Yang, Michael Walter, Michael Sommer and Matthias Müller
Recently, it has been shown that the sulfur load and subsequently the sulfur strand length of organo-sulfur networks prepared via inverse vulcanization for lithium organo-sulfur batteries impact the battery performance in terms of specific capacity and stability. In this work, we quantify the distribution of sulfur strand lengths evolving over the course of several charge–discharge cycles using operando X-ray absorption spectrometry. The results correlate the stability of sulfur strand length and (ir)reversibility of S-strand reduction and accompanied cleavage with battery cycling.
{"title":"Evolution of the sulfur strand length distribution in lithium organo-sulfur batteries monitored through operando X-ray absorption spectrometry","authors":"Konstantin Skudler, Rukiya Matsidik, Ayda Gholamhosseinian, Hongfei Yang, Michael Walter, Michael Sommer and Matthias Müller","doi":"10.1039/D5SE01115A","DOIUrl":"https://doi.org/10.1039/D5SE01115A","url":null,"abstract":"<p >Recently, it has been shown that the sulfur load and subsequently the sulfur strand length of organo-sulfur networks prepared <em>via</em> inverse vulcanization for lithium organo-sulfur batteries impact the battery performance in terms of specific capacity and stability. In this work, we quantify the distribution of sulfur strand lengths evolving over the course of several charge–discharge cycles using operando X-ray absorption spectrometry. The results correlate the stability of sulfur strand length and (ir)reversibility of S-strand reduction and accompanied cleavage with battery cycling.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 6822-6829"},"PeriodicalIF":4.1,"publicationDate":"2025-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se01115a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145652198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hou-Chin Cha, Shih-Han Huang, Chia-Feng Li, Feng-Yu Tsai, Wei-Fang Su and Yu-Ching Huang
Correction for ‘Advances and strategies in scalable coating techniques for flexible perovskite solar cells’ by Hou-Chin Cha et al., Sustainable Energy Fuels, 2025, https://doi.org/10.1039/D5SE00873E.
{"title":"Correction: Advances and strategies in scalable coating techniques for flexible perovskite solar cells","authors":"Hou-Chin Cha, Shih-Han Huang, Chia-Feng Li, Feng-Yu Tsai, Wei-Fang Su and Yu-Ching Huang","doi":"10.1039/D5SE90082D","DOIUrl":"https://doi.org/10.1039/D5SE90082D","url":null,"abstract":"<p >Correction for ‘Advances and strategies in scalable coating techniques for flexible perovskite solar cells’ by Hou-Chin Cha <em>et al.</em>, <em>Sustainable Energy Fuels</em>, 2025, https://doi.org/10.1039/D5SE00873E.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 23","pages":" 6563-6574"},"PeriodicalIF":4.1,"publicationDate":"2025-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/se/d5se90082d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145537634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Monodisperse PtCo bimetallic alloy nanoparticles (NPs) were successfully synthesized via a facile impregnation–reduction method utilizing oxidized carbon nanohorns (oxCNHs) as a high-surface-area support. The optimized Pt1.5Co-oxCNH catalyst demonstrated exceptional performance for hydrogen evolution via ammonia borane (AB) hydrolysis under mild conditions (298 K), achieving a high turnover frequency (TOF) of 445 molH2 molPt−1 min−1. This represents a 2.7-fold enhancement compared to the monometallic Pt-oxCNH benchmark and is accompanied by a significant reduction in the apparent activation energy. Synergistic electronic effects within the Pt1.5Co alloy were identified as critical to this performance boost. Furthermore, the unique nanoconfined pore structure of the oxCNH support effectively stabilized the PtCo NPs, minimizing aggregation and maintaining a small particle size, thereby maximizing accessible active sites and enhancing catalyst stability. The exceptional catalytic activity stems from the optimized electronic structure of Pt, modulated by localized electron density transfer via the Co alloying effect, coupled with strong metal–support interactions between the NPs and the functionalized oxCNH surface. This work provides a strategic design principle for developing highly active and durable heterogeneous catalysts for efficient hydrogen production.
{"title":"Dual engineering of electronic structure and nanoconfinement for high-efficiency ammonia borane hydrolysis over PtCo-oxCNH catalysts","authors":"Weixia Li, Wenjing Yi, Runzi Liao, Houfa Chen and Xinzheng Yue","doi":"10.1039/D5SE01247C","DOIUrl":"https://doi.org/10.1039/D5SE01247C","url":null,"abstract":"<p >Monodisperse PtCo bimetallic alloy nanoparticles (NPs) were successfully synthesized <em>via</em> a facile impregnation–reduction method utilizing oxidized carbon nanohorns (oxCNHs) as a high-surface-area support. The optimized Pt<small><sub>1.5</sub></small>Co-oxCNH catalyst demonstrated exceptional performance for hydrogen evolution <em>via</em> ammonia borane (AB) hydrolysis under mild conditions (298 K), achieving a high turnover frequency (TOF) of 445 mol<small><sub>H<small><sub>2</sub></small></sub></small> mol<small><sub>Pt</sub></small><small><sup>−1</sup></small> min<small><sup>−1</sup></small>. This represents a 2.7-fold enhancement compared to the monometallic Pt-oxCNH benchmark and is accompanied by a significant reduction in the apparent activation energy. Synergistic electronic effects within the Pt<small><sub>1.5</sub></small>Co alloy were identified as critical to this performance boost. Furthermore, the unique nanoconfined pore structure of the oxCNH support effectively stabilized the PtCo NPs, minimizing aggregation and maintaining a small particle size, thereby maximizing accessible active sites and enhancing catalyst stability. The exceptional catalytic activity stems from the optimized electronic structure of Pt, modulated by localized electron density transfer <em>via</em> the Co alloying effect, coupled with strong metal–support interactions between the NPs and the functionalized oxCNH surface. This work provides a strategic design principle for developing highly active and durable heterogeneous catalysts for efficient hydrogen production.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 23","pages":" 6470-6478"},"PeriodicalIF":4.1,"publicationDate":"2025-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145537670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Manish Ramesh Shingole, Siddhartha Kolay, Asheesh Kumar, P. Ruz, V. Sudarsan and Seemita Banerjee
Designing multimodal catalysts with high efficiency and durability remains a central challenge in clean energy research. High-entropy materials, composed of multiple principal elements, have recently emerged as promising candidate in catalysis owing to their tunable active sites, synergistic effects, and enhanced stability. In this study, a novel non-noble metals based high entropy metal–organic framework (HE-MOF) was synthesized and subsequently converted into a high-entropy alloy in carbon matrix (HEA@Carbon) through controlled thermal treatment under static hydrogen atmosphere. Detailed structural and compositional analyses were carried out using XRD, FTIR, Raman, SEM-EDX, and TEM to confirm the successful formation of the HEA phase with the preservation of the carbon morphology. The HEA@Carbon catalyst exhibited excellent catalytic performance for the hydrolysis of ammonia borane (AB), achieving a TOF value of 316 min−1 with an apparent activation energy (Ea) of 9.6 kJ mol−1, representing a nearly tenfold decrease in activation energy for AB hydrolysis compared to the non-catalytic reaction. The catalyst retained nearly identical catalytic activity over five consecutive cycles, demonstrating excellent durability. Importantly, the HEA@Carbon catalyst's inherent magnetic recoverability enables facile separation and reuse, with 96% catalyst recovery after the reusability test, underscoring its practical suitability for scalable hydrogen production. Beyond catalytic hydrogen production from chemical hydrides, HEA@Carbon exhibited notable electrocatalytic hydrogen evolution reaction (HER) activity with an overpotential of 400 mV at 10 mA cm−2 and a Tafel slope of 92 mV dec−1, together with the long-term operational stability. These results underscore the great potential of HEA embedded within a carbon matrix as a bifunctional catalyst for both chemical and electrochemical hydrogen generation, for next-generation hydrogen energy systems.
设计高效、耐用的多模态催化剂是清洁能源研究的核心挑战。由多个主元素组成的高熵材料,由于其可调节的活性位点、协同效应和增强的稳定性,最近在催化方面成为有希望的候选者。在本研究中,合成了一种新型的非贵金属高熵金属有机骨架(HE-MOF),并在静态氢气氛下通过控制热处理将其转化为碳基体(HEA@Carbon)的高熵合金。利用XRD、FTIR、Raman、SEM-EDX和TEM等手段对样品进行了详细的结构和成分分析,证实了HEA相的成功形成,并保留了碳的形貌。HEA@Carbon催化剂对氨硼烷(AB)的水解表现出优异的催化性能,TOF值为316 min−1,表观活化能(Ea)为9.6 kJ mol−1,与非催化反应相比,AB水解的活化能降低了近10倍。该催化剂在连续五个循环中几乎保持相同的催化活性,表现出优异的耐久性。重要的是,HEA@Carbon催化剂固有的磁性可回收性使其易于分离和重复使用,在可重复使用测试后,催化剂回收率为96%,强调了其可扩展制氢的实用性。除了化学氢化物催化制氢之外,HEA@Carbon还具有显著的电催化析氢反应(HER)活性,在10 mA cm−2下过电位为400 mV, Tafel斜率为92 mV dec−1,并且具有长期的运行稳定性。这些结果强调了嵌入在碳基体中的HEA作为下一代氢能系统化学和电化学制氢双功能催化剂的巨大潜力。
{"title":"Magnetically recoverable high-entropy alloy catalyst in carbon matrix for ammonia borane-driven hydrogen evolution and electrocatalytic hydrogen production","authors":"Manish Ramesh Shingole, Siddhartha Kolay, Asheesh Kumar, P. Ruz, V. Sudarsan and Seemita Banerjee","doi":"10.1039/D5SE01117E","DOIUrl":"https://doi.org/10.1039/D5SE01117E","url":null,"abstract":"<p >Designing multimodal catalysts with high efficiency and durability remains a central challenge in clean energy research. High-entropy materials, composed of multiple principal elements, have recently emerged as promising candidate in catalysis owing to their tunable active sites, synergistic effects, and enhanced stability. In this study, a novel non-noble metals based high entropy metal–organic framework (HE-MOF) was synthesized and subsequently converted into a high-entropy alloy in carbon matrix (HEA@Carbon) through controlled thermal treatment under static hydrogen atmosphere. Detailed structural and compositional analyses were carried out using XRD, FTIR, Raman, SEM-EDX, and TEM to confirm the successful formation of the HEA phase with the preservation of the carbon morphology. The HEA@Carbon catalyst exhibited excellent catalytic performance for the hydrolysis of ammonia borane (AB), achieving a TOF value of 316 min<small><sup>−1</sup></small> with an apparent activation energy (<em>E</em><small><sub>a</sub></small>) of 9.6 kJ mol<small><sup>−1</sup></small>, representing a nearly tenfold decrease in activation energy for AB hydrolysis compared to the non-catalytic reaction. The catalyst retained nearly identical catalytic activity over five consecutive cycles, demonstrating excellent durability. Importantly, the HEA@Carbon catalyst's inherent magnetic recoverability enables facile separation and reuse, with 96% catalyst recovery after the reusability test, underscoring its practical suitability for scalable hydrogen production. Beyond catalytic hydrogen production from chemical hydrides, HEA@Carbon exhibited notable electrocatalytic hydrogen evolution reaction (HER) activity with an overpotential of 400 mV at 10 mA cm<small><sup>−2</sup></small> and a Tafel slope of 92 mV dec<small><sup>−1</sup></small>, together with the long-term operational stability. These results underscore the great potential of HEA embedded within a carbon matrix as a bifunctional catalyst for both chemical and electrochemical hydrogen generation, for next-generation hydrogen energy systems.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 23","pages":" 6548-6562"},"PeriodicalIF":4.1,"publicationDate":"2025-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145537633","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}