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NiO composites with blackberry seed-derived activated carbon (NiO/BBSDAC) for the improved electrochemical behavior of lithium-ion battery anodes 黑莓籽源活性炭NiO复合材料(NiO/BBSDAC)用于改善锂离子电池阳极的电化学行为
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-28 DOI: 10.1039/D5SE00858A
Chandra Sekhar Bongu, V. Ganesh and Edreese H. Alsharaeh

To enhance the electrochemical performance of lithium-ion batteries (LIBs) in applications, nano NiO was created as an anode material in this work via a simple hydrothermal synthesis approach using a composite with bio-carbon (blackberry seeds derived activated carbon). NiO particles were evenly dispersed across the BBSDAC's surface, according to scanning electron microscopy (SEM) and transmission electron microscopy (TEM) studies. The resulting composite (NiO@10%-C) with micropores and mesopores showed potential for quick electron/ion transfer, electrolyte penetration to the electrode surface, and prevention of NiO volume expansion during the electrochemical study. In comparison to pristine NiO and the other two composite anode materials (NiO@5%-C and NiO@20%-C), the NiO@10%-C composite material exhibited good rate performance, long cycle life, and high reversibility when employed as an anode material for lithium-ion batteries. The NiO@10%-C material had a coulombic efficiency of 99.5% and a capacity of 807 mA h g−1 at a current density of 100 mA g−1 for up to 100 cycles. However, the pristine NiO, NiO@5%-C, and NiO@20%-C materials exhibited a capacity of 112, 207, and 458 mA h g−1, respectively. The exceptional performance of the NiO@10%-C electrode originated from the presence of BBSDAC on NiO, which accelerated the electron transfer and reduced the volume change of NiO during the lithiation and delithiation processes. Accordingly, it is thought that the BBSDAC can be used to enhance the electrochemical capabilities of different metal-oxide electrodes in rechargeable batteries.

为了提高锂离子电池(LIBs)在应用中的电化学性能,本研究采用生物碳(黑莓籽衍生活性炭)复合材料,通过简单的水热合成方法制备了纳米NiO作为阳极材料。根据扫描电镜(SEM)和透射电镜(TEM)的研究,NiO颗粒均匀地分散在BBSDAC的表面。所得复合材料(NiO@10% c)具有微孔和介孔,在电化学研究中具有快速电子/离子转移、电解质渗透到电极表面和防止NiO体积膨胀的潜力。与原始NiO和其他两种复合负极材料(NiO@5% c和NiO@20% c)相比,NiO@10% c复合材料作为锂离子电池负极材料具有良好的倍率性能、长循环寿命和高可逆性。NiO@10% c材料的库仑效率为99.5%,在100 mA g - 1电流密度下的容量为807 mA h g - 1,最多可循环100次。然而,原始NiO、NiO@5% c和NiO@20% c材料的容量分别为112、207和458 mA h g−1。NiO@10% c电极的优异性能源于NiO上BBSDAC的存在,它加速了NiO在锂化和锂化过程中的电子转移,减少了NiO的体积变化。因此,我们认为该材料可用于提高可充电电池中不同金属氧化物电极的电化学性能。
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引用次数: 0
Catalytic CO2 hydrogenation to sustainable aviation fuel: mechanisms and pathways to net-zero 催化二氧化碳加氢生产可持续航空燃料:实现净零排放的机制和途径
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-28 DOI: 10.1039/D5SE01236H
Nur'ain Nadia Shapril, Yasmin Abdul Wahab, Durga Devi Suppiah and Mohd Rafie Johan

Aviation's 2.5% contribution to global CO2 emissions necessitates scalable, sustainable jet fuel alternatives. This review addresses the gap in comprehensive CO2-to-Sustainable Aviation Fuel (SAF) analyses by examining Power-to-Liquid (PtL) technologies, focusing on CO2 hydrogenation via Fischer–Tropsch synthesis, methanol-to-jet (MtJ), and direct hydrogenation pathways. We analyze recent advances in bifunctional catalysts and tandem mechanisms, achieving 21–57% energy efficiencies and jet fuel costs of 2–9 € kg−1. A phased 2050 commercialization roadmap aligns technology readiness levels with policies like EU's ReFuelEU. Case studies (Haru Oni, Synhelion, OXCCU) highlight real-world progress, while life cycle assessments reveal carbon intensities of 10–83 gCO2e MJ−1. Challenges, including catalyst deactivation and green hydrogen scalability, are evaluated alongside opportunities in AI-driven catalyst design and modular reactors. By integrating catalysis, techno-economics, and policy, this work guides researchers, industry, and policymakers toward net-zero aviation.

航空业占全球二氧化碳排放量的2.5%,因此需要可扩展的、可持续的航空燃料替代品。本文通过考察动力制液(PtL)技术,重点研究了通过费托合成、甲醇制喷气(MtJ)和直接加氢途径进行的二氧化碳加氢,填补了二氧化碳到可持续航空燃料(SAF)综合分析的空白。我们分析了双功能催化剂和串联机制的最新进展,实现了21-57%的能源效率和2-9€kg - 1的航空燃料成本。分阶段的2050年商业化路线图将技术准备水平与欧盟的燃料燃料联盟等政策保持一致。案例研究(Haru Oni, Synhelion, OXCCU)强调了现实世界的进展,而生命周期评估显示碳强度为10-83 gCO2e MJ - 1。与人工智能驱动的催化剂设计和模块化反应器的机遇一起,评估了包括催化剂失活和绿色氢可扩展性在内的挑战。通过整合催化、技术经济学和政策,这项工作指导研究人员、行业和政策制定者实现航空零净。
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引用次数: 0
Bifunctional PGM-free electrocatalysts for seawater batteries 海水电池用无pgm双功能电催化剂
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-28 DOI: 10.1039/D5SE00907C
Pedro Pablo Machado Pico, Jorge Montero, Akiko Tsurumaki, Stefano Passerini and Maria Assunta Navarra

Seawater batteries (SWBs) are an emerging energy storage solution that leverages the abundant and cost-effective sodium ions present in seawater. However, their performance is often constrained by the sluggish kinetics of the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) at the seawater cathode. To overcome these limitations, a series of platinum group metal (PGM)-free bifunctional electrocatalysts was developed to enhance OER/ORR catalytic activity and overall power performance. Metal-doped nitrogen carbon nanoparticles (M–N–C), namely FeNiNC, FeNC, and NiNC, were synthesized via a simple precipitation method followed by heat treatment, yielding active metal sites dispersed in an amorphous carbon structure. The use of low-cost biomass derived from hazelnut shells as a carbon-based material, modified with Fe and/or Ni, resulted in a highly efficient catalyst. In particular, FeNiNC exhibited an ORR activity of 0.81 V vs. RHE at half-potential and an OER activity of 1.57 V vs. RHE at a current density of 10 mA cm−2. Electrochemical characterization demonstrated that SWBs incorporating the FeNiNC catalyst achieved enhanced power output and cycling stability, maintaining performance for 350 hours.

海水电池(swb)是一种新兴的能源存储解决方案,它利用了海水中丰富且具有成本效益的钠离子。然而,它们的性能往往受到海水阴极析氧反应(OER)和氧还原反应(ORR)动力学迟缓的制约。为了克服这些限制,开发了一系列不含铂族金属(PGM)的双功能电催化剂,以提高OER/ORR的催化活性和整体功率性能。采用简单沉淀法和热处理法制备了金属掺杂氮碳纳米颗粒(M-N-C),即FeNiNC、FeNC和NiNC,得到了分散在非晶碳结构中的活性金属位。利用从榛子壳中提取的低成本生物质作为碳基材料,用铁和/或镍改性,产生了高效的催化剂。特别是,FeNiNC在半电位下的ORR活性为0.81 V,在电流密度为10 mA cm−2时的OER活性为1.57 V。电化学表征表明,加入FeNiNC催化剂的swb获得了更高的功率输出和循环稳定性,可保持350小时的性能。
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引用次数: 0
Life cycle greenhouse gas emissions and carbon intensity of U.S. fuel use and projection for the next 10 years-based on built capacity and expansion plans 美国燃料使用的生命周期温室气体排放和碳强度,以及基于已建成产能和扩张计划的未来10年预测
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-27 DOI: 10.1039/D5SE00769K
Tai-Yuan Huang, Doris Oke and Troy R. Hawkins

The U.S. Inflation Reduction Act of 2022 supports biofuel production expansion through the 45Z clean fuel production tax credit, replacing previous 40A and 40B credits. This follows on the Renewable Fuel Standard from the Energy Policy Act of 2005 and its expansion in 2007. States like California, Oregon, and Washington also offer clean fuel credits. Meanwhile, federal agencies, including the U.S. Department of Energy, have advanced alternative fuel technologies through research and development funding. The surging interest in the biofuel industry has spurred the demand for biofuel supplies in the markets, although achieving profitability for advanced biofuels and low-carbon e-fuels remains challenging. This study aims to track U.S. alternative fuel production capacity expansion plans over the next 10 years and estimate impacts on greenhouse gas (GHG) emissions. By tracking built capacity and industry announcements of planned expansion, this study complements other studies which use models to predict changes in energy technologies and the associated GHG implications. Modeled projections of future technologies are often criticized for over or underestimating the cost and potential role of new technologies. The study focuses on sustainable aviation fuel, renewable diesel, ethanol, biodiesel, and renewable natural gas. Using facility-level data, we conducted a bottom-up analysis linking biofuel production pathways with corresponding pathways and parameterizations in the Argonne R&D GREET model. Results indicate that biofuel capacity could reach 3.8 exajoules in 2035, potentially reducing U.S. GHG emissions by 179 million tonnes, including the full life cycle. This corresponds to a 20% reduction in transportation and 5% in industry sector emissions by 2035, or a 3.6% reduction in economy-wide emissions. Overall, this study shows that while biofuel production capacity in the U.S. is expanding, the capacities remain limited compared to fuel demand. Uncertainty regarding the durability and extension of incentives may be dampening the pace of growth. Meanwhile, demonstrating the commercial potential for alternative fuels and climbing the learning curve for new technologies could lead to an increased pace of expansion in later years. This study offers insights for bioenergy stakeholders, highlighting biofuel technologies' contribution to U.S. energy system and emissions reduction over time based on producers' plans.

美国《2022年通货膨胀减少法案》通过45Z清洁燃料生产税收抵免来支持生物燃料生产扩张,取代之前的40A和40B抵免。这是继2005年能源政策法案的可再生燃料标准及其在2007年的扩展之后。加利福尼亚、俄勒冈和华盛顿等州也提供清洁燃料信用额度。与此同时,包括美国能源部在内的联邦机构通过研发资金推动了替代燃料技术的发展。尽管实现先进生物燃料和低碳电子燃料的盈利仍然具有挑战性,但对生物燃料行业的兴趣激增刺激了市场对生物燃料供应的需求。本研究旨在追踪美国未来10年替代燃料产能扩张计划,并估计其对温室气体排放的影响。通过跟踪已建成产能和行业宣布的扩张计划,本研究补充了其他使用模型预测能源技术变化和相关温室气体影响的研究。对未来技术的建模预测经常因高估或低估新技术的成本和潜在作用而受到批评。这项研究的重点是可持续航空燃料、可再生柴油、乙醇、生物柴油和可再生天然气。利用设施级数据,我们进行了自下而上的分析,将生物燃料生产途径与Argonne R&;D GREET模型中的相应途径和参数化联系起来。结果表明,到2035年,生物燃料的产能可能达到3.8焦耳,包括整个生命周期在内,可能会使美国的温室气体排放量减少1.79亿吨。这相当于到2035年,交通运输部门的排放量减少20%,工业部门的排放量减少5%,或者整个经济的排放量减少3.6%。总的来说,这项研究表明,虽然美国的生物燃料生产能力正在扩大,但与燃料需求相比,产能仍然有限。激励措施的持久性和延伸性的不确定性可能会抑制经济增长的步伐。与此同时,展示替代燃料的商业潜力和对新技术的学习曲线的攀升可能会导致未来几年扩张的步伐加快。这项研究为生物能源利益相关者提供了见解,强调了生物燃料技术对美国能源系统的贡献,以及基于生产商计划的长期减排。
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引用次数: 0
Utilizing nature's endowment: artificial leaf concept for methane activation to C–C coupled ethanol or ethylene 利用自然禀赋:人工叶片概念甲烷活化成碳-碳偶联乙醇或乙烯
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-27 DOI: 10.1039/D5SE01178G
Subhashree S. Kanungo, Abhaya Kumar Mishra, Mangaladasan J. Avani, Himanshu Bajpai, Kranti N. Salgaonkar, Bharathkumar H. Javaregowda and Chinnakonda S. Gopinath

Methane activation (MA) to platform chemicals under ambient conditions still remains an open challenge to be fully realised. The present work shows the fabrication of CeVO4 quantum dots (CV-QDs) by a bottom-up approach; they are assembled from Ce3+ and metavanadate ions, and structurally and electronically integrated into the micro-/meso-pores of TiO2 (CV-QD-TiO2 (CVT)), demonstrating the conversion of MA to ethanol/ethylene by visible light-driven photocatalysis. CV-QDs in confined pores modify the quantum confinement effects and are characterized by physicochemical methods. The current synthetic strategy is potentially scalable and results in sub-quadrillion heterojunctions in a 1 mg CVT photoanode spread over 1 cm2. MA with CVT under one-sun conditions demonstrates ∼100% selectivity to ethanol, yielding 4.36 μmol h−1 cm−2, with a solar-to-fuel efficiency (STFE) of 0.56. Further, by employing a co-catalyst, significant STFE (5.08) and yield (39.5 μmol h−1 cm−2) are achieved selectively towards ethylene. A deliberate addition of methanol increases the rate of ethanol production by 17.2 times, indicating that the methyl-methoxy interaction is the origin of C–C coupling. Weight is normalized to a gram of CV-QDs in a large area CVT photoanode to yield 109 mmol h−1 gCV-QD−1 of ethanol and 988 mmol h−1 gCV-QD−1 of ethylene. Enhanced activity and selectivity towards the C2-product is attributed to band-edge modulation and trillions of heterojunctions, which in turn facilitate charge separation and charge transfer for effective charge utilisation at redox sites.

在环境条件下,甲烷对平台化学物质的活化(MA)仍然是一个有待充分实现的挑战。本研究展示了用自下而上的方法制备CeVO4量子点(CV-QDs);它们由Ce3+和偏氰酸盐离子组装而成,并在结构上和电子上集成到TiO2 (CV-QD-TiO2 (CVT))的微孔/介孔中,证明了可见光驱动光催化将MA转化为乙醇/乙烯。封闭孔隙中的CV-QDs修饰了量子约束效应,并用物理化学方法对其进行了表征。目前的合成策略具有潜在的可扩展性,并且在1mg CVT光阳极中分布在1cm2上,可产生亚千万亿异质结。在单太阳条件下,具有CVT的MA对乙醇的选择性为100%,产率为4.36 μmol h−1 cm−2,太阳能-燃料效率(STFE)为0.56。此外,通过使用助催化剂,选择性地获得了显著的STFE(5.08)和产率(39.5 μmol h−1 cm−2)。故意添加甲醇可使乙醇的产率提高17.2倍,表明甲基-甲氧基相互作用是C-C偶联的起源。在大面积CVT光阳极中,将重量归一化为克CV-QDs,得到109 mmol h−1 gCV-QD−1乙醇和988 mmol h−1 gCV-QD−1乙烯。对c2产物增强的活性和选择性归因于带边调制和数万亿个异质结,这反过来促进了电荷分离和电荷转移,从而在氧化还原位点有效利用电荷。
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引用次数: 0
Hydrogen fuel cells: technical, economic, and policy pathways toward net-zero integration 氢燃料电池:实现净零整合的技术、经济和政策途径
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-27 DOI: 10.1039/D5SE01080B
Shlok Sahu, Ritika Kanwal, Ishika Ratnawat, Afkham Mir and Iyman Abrar

Hydrogen fuel cells (HFCs) present a viable clean energy solution but face significant economic and technical challenges. High costs, particularly from platinum-based catalysts and energy-intensive hydrogen production, hinder large-scale adoption. Green hydrogen, produced via renewable-powered electrolysis, remains expensive (∼$5.84 per kg), while infrastructure gaps and competition from battery electric vehicles further impede deployment. Technological barriers include catalyst degradation, membrane durability (e.g., Nafion in PEMFCs), and electrode design limitations. Emerging alternatives—such as palladium alloys, non-precious metal catalysts (M–N–C), and reinforced membranes—show promise but struggle with scalability and performance. System integration complexities, including thermal management and hydrogen storage, add to these challenges. Lifecycle assessments reveal that platinum accounts for ∼91% of MEA costs, while hydrogen production emissions vary widely (30–50 kg CO2 per kg in Australia vs. 5–10 kg CO2 per kg in Italy by 2030). Despite this, HFCs offer substantial decarbonization potential, particularly in heavy transport, with projected emission reductions of up to 67% by 2050. Future advancements hinge on AI-driven optimization, novel materials (e.g., MOFs for storage), and hybrid system designs. Policy support and infrastructure investment are critical to overcome the dilemma of supply and demand. This review specifically focuses on the significant gaps present in the existing literature by offering a thorough, multidisciplinary assessment that incorporates the latest developments in catalyst and membrane technology, comprehensive cost and lifecycle evaluations, and innovative AI-driven system optimization methods. In contrast to previous studies that predominantly emphasize isolated technical or economic factors, this paper distinctly merges technical, economic, environmental, and policy aspects to provide a comprehensive understanding of the scalability and sustainable integration of hydrogen fuel cells. By underscoring specific performance ranges, economic comparisons, and statistics on emission reduction, this review presents strategic insights that are crucial for researchers, policymakers, and industry leaders who are striving to expedite the transition to a hydrogen economy.

氢燃料电池(hfc)是一种可行的清洁能源解决方案,但面临着重大的经济和技术挑战。高昂的成本,特别是铂基催化剂和能源密集型制氢的成本,阻碍了大规模采用。通过可再生能源电解生产的绿色氢仍然昂贵(每公斤约5.84美元),而基础设施差距和来自电池电动汽车的竞争进一步阻碍了部署。技术障碍包括催化剂降解、膜耐久性(例如pemfc中的Nafion)和电极设计限制。新兴的替代品,如钯合金、非贵金属催化剂(M-N-C)和增强膜,都表现出了希望,但在可扩展性和性能方面存在困难。系统集成的复杂性,包括热管理和储氢,增加了这些挑战。生命周期评估显示,铂金占MEA成本的91%,而氢气生产的排放量差异很大(到2030年,澳大利亚每公斤30-50公斤二氧化碳,意大利每公斤5-10公斤二氧化碳)。尽管如此,氢氟碳化物仍具有巨大的脱碳潜力,特别是在重型运输领域,预计到2050年将减少高达67%的排放量。未来的发展取决于人工智能驱动的优化、新型材料(例如用于存储的mof)和混合系统设计。政策支持和基础设施投资是解决供需困境的关键。本综述通过提供全面的多学科评估,结合催化剂和膜技术的最新发展,综合成本和生命周期评估以及创新的人工智能驱动的系统优化方法,特别关注现有文献中存在的重大空白。与以往的研究主要强调孤立的技术或经济因素不同,本文明确地将技术,经济,环境和政策方面结合起来,全面了解氢燃料电池的可扩展性和可持续整合。通过强调具体的性能范围、经济比较和减排统计数据,本综述为正在努力加速向氢经济过渡的研究人员、政策制定者和行业领导者提供了至关重要的战略见解。
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引用次数: 0
Constructing stable cathode interfaces with halide–sulfide dual electrolytes for all-solid-state lithium batteries with enhanced electrochemical performance 构建稳定的卤化物-硫化物双电解质阴极界面,提高全固态锂电池的电化学性能
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-27 DOI: 10.1039/D5SE01037C
Wenzhuang Liu, Jiahao Li, Jinghua Wu and Xiayin Yao

Interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes remains a major bottleneck hindering the development of high-performance all-solid-state lithium batteries (ASSLBs). Conventional coating materials often suffer from low ionic conductivity and poor mechanical deformability, necessitating complex processing or additional interlayers. Halide electrolytes offer good stability, ionic conductivity, and softness, but their poor reductive stability with lithium metal limits their use as standalone solid electrolytes in full cells. In this work, we propose a dual-electrolyte composite cathode strategy by introducing a halide electrolyte, Li3InCl6 (LIC), as a functional surface coating for LiNi0.8Co0.1Mn0.1O2 (NCM). The nanosized Li3InCl6 particles synthesized by freeze-drying exhibit high ionic conductivity and uniform particle size distribution, making them effective as interfacial buffer layers. The optimized 15% LIC@NCM composite cathode delivers a high initial capacity of 189 mA h g−1 with a coulombic efficiency of 84.4% at 0.1 C, along with remarkable cycling stability, retaining 114 mA h g−1 after 250 cycles at 0.5 C. Comprehensive electrochemical and spectroscopic analyses confirm that the Li3InCl6 coating effectively mitigates interfacial degradation, suppresses side reactions, and facilitates ion transport across the composite interface. This study offers a facile and scalable interface engineering strategy using halide electrolytes to simultaneously enhance lithium-ion transport and interfacial stability in sulfide-based ASSLBs.

富镍层状氧化物阴极与硫化物电解质之间的界面不稳定性一直是阻碍高性能全固态锂电池(ASSLBs)发展的主要瓶颈。传统的涂层材料通常离子电导率低,机械变形能力差,需要复杂的加工或额外的中间层。卤化物电解质具有良好的稳定性、离子导电性和柔软性,但它们与锂金属的还原稳定性差,限制了它们在完整电池中作为独立固体电解质的使用。在这项工作中,我们提出了一种双电解质复合阴极策略,通过引入卤化物电解质Li3InCl6 (LIC)作为LiNi0.8Co0.1Mn0.1O2 (NCM)的功能表面涂层。冻干法制备的Li3InCl6纳米颗粒具有较高的离子电导率和均匀的粒径分布,可作为界面缓冲层。优化后的15% LIC@NCM复合阴极在0.1℃下具有189 mA h g−1的高初始容量和84.4%的库伦效率,以及出色的循环稳定性,在0.5℃下循环250次后仍保持114 mA h g−1。综合电化学和光谱分析证实,Li3InCl6涂层有效地减轻了界面降解,抑制了副反应,并促进了离子在复合界面上的传输。这项研究提供了一种简单且可扩展的界面工程策略,使用卤化物电解质同时增强硫化物基assb中的锂离子传输和界面稳定性。
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引用次数: 0
Upcycling polyethylene into diesel-range hydrocarbons over Ru catalysts confined in thermally stable mesoporous N-doped carbon 热稳定中孔n掺杂碳催化剂上的Ru催化剂将聚乙烯升级为柴油级碳氢化合物
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-24 DOI: 10.1039/D5SE01013F
Shitong Yu, Zhenghang Ren, Kaige Wang, Rui Xiao, Zhicheng Luo and Huiyan Zhang

Plastic waste management is a critical sustainability challenge, but it also offers an opportunity to produce clean fuels from carbon-rich materials. In this study, we report a ruthenium catalyst supported on thermally stable mesoporous nitrogen-doped carbon (Ru/NAC) for the solvent-free hydrogenolysis of polyethylene into diesel-range hydrocarbons. The catalyst features ultrasmall Ru nanoparticles (∼1.48 nm), uniformly dispersed and stabilized by Ru–N coordination within an ordered mesoporous carbon framework. This architecture enhances polymer–catalyst interactions and enables controlled C–C bond cleavage. Under mild conditions (300 °C, 3 MPa H2), Ru/NAC achieves a high liquid yield (86.5%) with 90.4% selectivity toward C8–C22 alkanes and a productivity of 391.1 gp gRu−1 h−1. Mechanistic studies, including 13C solid-state NMR and in situ Diffuse Reflectance Infrared Fourier Transform spectroscopy, reveal that mesopore confinement and homogeneous metal dispersion synergistically promote selective depolymerization pathways. This strategy offers a practical and scalable route for transforming polyolefin waste into sustainable fuel-range hydrocarbons, advancing circular energy systems.

塑料废物管理是一个关键的可持续性挑战,但它也提供了一个从富含碳的材料生产清洁燃料的机会。在这项研究中,我们报道了一种热稳定的介孔氮掺杂碳(Ru/NAC)负载的钌催化剂,用于无溶剂氢解聚乙烯成柴油烃类。催化剂具有超小的Ru纳米颗粒(~ 1.48 nm),在有序的介孔碳框架内均匀分散并通过Ru - n配位稳定。这种结构增强了聚合物-催化剂的相互作用,并使控制C-C键的裂解成为可能。在温和条件下(300℃,3 MPa H2), Ru/NAC对C8-C22烷烃的收率为86.5%,选择性为90.4%,产率为391.1 gp gRu−1 h−1。机制研究,包括13C固体核磁共振和原位漫反射红外傅立叶变换光谱,揭示了介孔限制和均匀金属分散协同促进选择性解聚途径。这一战略为将聚烯烃废物转化为可持续燃料范围的碳氢化合物提供了一条实用且可扩展的途径,促进了循环能源系统的发展。
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引用次数: 0
Unveiling atomic-scale mechanisms of tantalum-based 2D materials for high-performance Li–S batteries 揭示用于高性能锂电池的钽基二维材料的原子尺度机制
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-24 DOI: 10.1039/D5SE01110H
Shrish Nath Upadhyay and Jayant K. Singh

The development of effective electrocatalysts is vital for advancing lithium–sulfur (Li–S) batteries, particularly in addressing sluggish redox kinetics and the polysulfide shuttle effect. In this study, we systematically investigate the catalytic behavior of three tantalum-based two-dimensional (2D) monolayers, TaS2, Ta2C, and hybrid Ta2S2C, using first-principles calculations. All three systems exhibit excellent thermal and structural stability, confirmed by geometry optimizations and ab initio molecular dynamics (AIMD) simulations. Electronic structure analyses indicate metallic character in each case. Adsorption energy analysis reveals that TaS2 binds strongly with Li2S4 (−2.60 eV), Li2S2 (−2.94 eV), and Li2S (−3.93 eV), in sharp contrast to Ta2C, which shows weak binding (e.g., +1.63 eV for Li2S4). Ta2S2C exhibits intermediate strength (−2.02 eV for Li2S2). Bader charge analysis further confirms significant electron redistribution during polysulfide anchoring, with up to 1.28|e| transferred on TaS2. Importantly, free energy profiles along the sulfur reduction reaction (SRR) pathway demonstrate that the critical Li2S2 → Li2S conversion step proceeds with a remarkably low barrier of 0.08 eV on TaS2, compared to 0.70 eV on Ta2C and 0.59 eV on Ta2S2C. These findings demonstrate that surface composition and coordination environments have a significant impact on catalytic performance. Overall, TaS2 emerges as the most promising sulfur host, combining superior conductivity, strong polysulfide adsorption, and ultrafast catalytic kinetics, while Ta2S2C offers balanced anchoring and activity. This work provides atomic-scale insights for the rational design of advanced 2D electrocatalysts for high-performance Li–S batteries.

开发有效的电催化剂对于推进锂硫电池的发展至关重要,特别是在解决缓慢的氧化还原动力学和多硫化物穿梭效应方面。在这项研究中,我们使用第一性原理计算系统地研究了三种钽基二维(2D)单层,TaS2, Ta2C和杂化Ta2S2C的催化行为。经过几何优化和从头算分子动力学(AIMD)模拟,这三种体系均表现出优异的热稳定性和结构稳定性。电子结构分析表明每种材料都具有金属特征。吸附能分析表明,TaS2与Li2S4(−2.60 eV)、Li2S2(−2.94 eV)和Li2S(−3.93 eV)结合较强,与Ta2C的结合较弱(Li2S4 +1.63 eV)形成鲜明对比。Ta2S2C具有中等强度(Li2S2为- 2.02 eV)。Bader电荷分析进一步证实了在多硫化物锚定过程中显著的电子再分配,在TaS2上转移了高达1.28 bb100 e|。重要的是,沿硫还原反应(SRR)途径的自由能谱表明,Li2S2→Li2S的关键转化步骤在TaS2上以0.08 eV的极低势垒进行,而Ta2C和Ta2S2C的势垒分别为0.70 eV和0.59 eV。这些发现表明,表面组成和配位环境对催化性能有显著影响。总的来说,TaS2是最有前途的硫宿主,具有优异的导电性、强的多硫吸附和超快的催化动力学,而Ta2S2C具有平衡的锚定和活性。这项工作为高性能锂硫电池的先进二维电催化剂的合理设计提供了原子尺度的见解。
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引用次数: 0
Visible-light-driven green hydrogen and hydrogen peroxide production using a 2D porous organic polymer engineered with 2D SnS2 利用2D SnS2设计的二维多孔有机聚合物生产可见光驱动的绿色氢气和过氧化氢
IF 4.1 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-10-22 DOI: 10.1039/D5SE01138H
Mainak Sarkar, Pekham Chakrabortty, R. V. Singh, Mrinal R. Pai, Mahboob Alam, Sk. Manirul Islam and Ahmed Mohamed Tawfeek

The transformation of solar radiation into chemical energy or valuable chemical compounds has garnered significant research interest, particularly in light of the global energy crisis. Hydrogen and hydrogen peroxide serve as sustainable energy sources in fuel cells, producing electricity with zero carbon emissions. Recently, the eco-friendly synthesis of H2 and H2O2 from water and oxygen using porous organic polymers (POPs) as photocatalysts has drawn considerable attention. However, their applications have been limited due to low absorption of visible light and the rapid recombination of photoinduced charge carriers, while noble metal co-catalysts remain essential in all POP-based photocatalysts to achieve high rates of hydrogen evolution and hydrogen peroxide production, as well as to enhance charge separation in semiconductor photocatalysts. In this study, we demonstrate a more effective heterojunction photocatalyst—2D–2D SnS2@TAPA-BPDA—which has a significant effect on photocatalytic H2 evolution and H2O2 production. When exposed to visible light, the SnS2@TAPA-BPDA composite achieves a hydrogen evolution rate of 1818.8 μmol h−1 g−1, which is approximately 30 times higher than that of the bare TAPA-BPDA POP. Similarly, for hydrogen peroxide production, the same catalyst reaches 3013.3 μmol h−1 g−1, nearly 14 times greater than the bare catalyst. These results highlight the significant enhancement in photocatalytic H2 evolution and H2O2 generation, leading to highly effective solar-to-chemical energy conversion.

太阳辐射转化为化学能或有价值的化合物已经引起了重大的研究兴趣,特别是在全球能源危机的情况下。氢和过氧化氢作为燃料电池的可持续能源,产生零碳排放的电力。近年来,利用多孔有机聚合物(POPs)作为光催化剂,从水和氧中环保合成H2和H2O2的研究备受关注。然而,由于可见光的低吸收和光致电荷载流子的快速重组,它们的应用受到限制,而贵金属共催化剂仍然是所有基于pop的光催化剂中必不可少的,以实现高速率的析氢和过氧化氢生产,以及增强半导体光催化剂中的电荷分离。在这项研究中,我们展示了一种更有效的异质结光催化剂- 2d - 2d SnS2@TAPA-BPDA -它对光催化H2的生成和H2O2的产生有显著的影响。当暴露在可见光下,SnS2@TAPA-BPDA复合材料的析氢速率为1818.8 μmol h−1 g−1,比裸材料的析氢速率高约30倍。同样,对于过氧化氢的生产,同样的催化剂达到3013.3 μmol h−1 g−1,几乎是裸催化剂的14倍。这些结果突出了光催化H2演化和H2O2生成的显著增强,从而实现了高效的太阳能-化学能转换。
{"title":"Visible-light-driven green hydrogen and hydrogen peroxide production using a 2D porous organic polymer engineered with 2D SnS2","authors":"Mainak Sarkar, Pekham Chakrabortty, R. V. Singh, Mrinal R. Pai, Mahboob Alam, Sk. Manirul Islam and Ahmed Mohamed Tawfeek","doi":"10.1039/D5SE01138H","DOIUrl":"https://doi.org/10.1039/D5SE01138H","url":null,"abstract":"<p >The transformation of solar radiation into chemical energy or valuable chemical compounds has garnered significant research interest, particularly in light of the global energy crisis. Hydrogen and hydrogen peroxide serve as sustainable energy sources in fuel cells, producing electricity with zero carbon emissions. Recently, the eco-friendly synthesis of H<small><sub>2</sub></small> and H<small><sub>2</sub></small>O<small><sub>2</sub></small> from water and oxygen using porous organic polymers (POPs) as photocatalysts has drawn considerable attention. However, their applications have been limited due to low absorption of visible light and the rapid recombination of photoinduced charge carriers, while noble metal co-catalysts remain essential in all POP-based photocatalysts to achieve high rates of hydrogen evolution and hydrogen peroxide production, as well as to enhance charge separation in semiconductor photocatalysts. In this study, we demonstrate a more effective heterojunction photocatalyst—2D–2D SnS<small><sub>2</sub></small>@TAPA-BPDA—which has a significant effect on photocatalytic H<small><sub>2</sub></small> evolution and H<small><sub>2</sub></small>O<small><sub>2</sub></small> production. When exposed to visible light, the SnS<small><sub>2</sub></small>@TAPA-BPDA composite achieves a hydrogen evolution rate of 1818.8 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>, which is approximately 30 times higher than that of the bare TAPA-BPDA POP. Similarly, for hydrogen peroxide production, the same catalyst reaches 3013.3 μmol h<small><sup>−1</sup></small> g<small><sup>−1</sup></small>, nearly 14 times greater than the bare catalyst. These results highlight the significant enhancement in photocatalytic H<small><sub>2</sub></small> evolution and H<small><sub>2</sub></small>O<small><sub>2</sub></small> generation, leading to highly effective solar-to-chemical energy conversion.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 23","pages":" 6479-6491"},"PeriodicalIF":4.1,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145537671","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}
引用次数: 0
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