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Asymmetric active sites originate from high-entropy metal selenides by joule heating to boost electrocatalytic water oxidation 通过焦耳加热从高熵金属硒化物中产生不对称活性位点,促进电催化水氧化
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-25 DOI: 10.1016/j.joule.2024.06.004
Fangren Qian, Lishan Peng, Dengfeng Cao, Wei Jiang, Chengsi Hu, Jiabao Huang, Xinping Zhang, Jiahui Luo, Shuangming Chen, Xiaojun Wu, Li Song, Qingjun Chen

High-entropy materials (HEMs) have garnered tremendous attention for electrocatalytic water oxidation because of their extraordinary properties. Nevertheless, scant attention has been directed toward comprehending the origin of their excellent activity and intricate atomic arrangements. Herein, we demonstrate the synthesis of high-entropy metal selenides (HEMSs) using a rapid joule-heating method, effectively circumventing the immiscibility challenges inherent in combining multiple metal elements. This achievement is collectively verified by a convergence of diverse analytical techniques encompassing quasi in situ X-ray absorption spectroscopy and operando attenuated total reflectance infrared spectroscopy. The HEMS exhibits a low overpotential of 222 mV at 10 mA cm−2 and extraordinary durability with negligible degradation over a 1,000 h durability test at 10 mA cm−2 and 500 h at 100 mA cm−2. Further, our theoretical investigations establish the pronounced mechanism of asymmetric Cu-Co-Ni active units in HEMS by manipulating the interaction of oxygen-containing intermediates, which leads to enhanced OER activity and durability.

高熵材料(HEMs)因其非凡的特性,在电催化水氧化方面获得了极大的关注。然而,人们很少关注其卓越活性和复杂原子排列的起源。在本文中,我们展示了利用快速焦耳加热法合成高熵金属硒化物(HEMSs)的过程,有效地规避了多种金属元素结合所固有的不溶性难题。准原位 X 射线吸收光谱和操作衰减全反射红外光谱等多种分析技术的融合共同验证了这一成果。在 10 mA cm-2 条件下,HEMS 的过电位很低,仅为 222 mV;在 10 mA cm-2 条件下,HEMS 的耐久性测试时间为 1,000 小时,在 100 mA cm-2 条件下,HEMS 的耐久性测试时间为 500 小时,降解几乎可以忽略不计。此外,我们的理论研究通过操纵含氧中间体的相互作用,确立了 HEMS 中不对称铜-铜-镍活性单元的显著机理,从而提高了 OER 的活性和耐用性。
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引用次数: 0
Domestic-first, climate second? Global consequences of the Inflation Reduction Act 国内第一,气候第二?减少通货膨胀法》的全球影响
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-21 DOI: 10.1016/j.joule.2024.06.001
Bessie Noll, Bjarne Steffen, Tobias S. Schmidt

Bessie Noll is a post doctoral researcher at the Energy and Technology Policy Group at ETH Zurich. Her research focuses on the effects of policy intervention on the development of clean energy technologies and transitional outcomes of modern energy systems. She holds a master’s degree in mechanical engineering from Stanford University and a PhD in energy and technology policy from ETH Zurich.

Bjarne Steffen is assistant professor and head of ETH Zurich’s Climate Finance and Policy Group. His research addresses the impact of public policy interventions on technological change in the energy sector, with a particular focus on the role of financial actors in reallocating capital. He holds a master’s degree in economics from the University of Mannheim and a PhD in energy economics from the University of Duisburg-Essen.

Tobias Schmidt is ETH Zurich’s professor of energy and technology policy and directs the Institute of Science, Technology, and Policy. His research focuses on the interaction of public policy and its underlying politics with technological change in energy-related sectors. He holds a master’s degree in electrical engineering from TU Munich and a doctorate from ETH Zurich.

贝西-诺尔(Bessie Noll)是苏黎世联邦理工学院能源与技术政策小组的博士后研究员。她的研究重点是政策干预对清洁能源技术发展和现代能源系统过渡成果的影响。她拥有斯坦福大学机械工程硕士学位和苏黎世联邦理工学院能源与技术政策博士学位。Bjarne Steffen 是苏黎世联邦理工学院助理教授兼气候金融与政策组组长。他的研究涉及公共政策干预对能源领域技术变革的影响,尤其关注金融参与者在重新分配资本方面的作用。托比亚斯-施密特(Tobias Schmidt)是苏黎世联邦理工学院的能源和技术政策教授,同时也是科学、技术和政策研究所的所长。他的研究重点是公共政策及其背后的政治与能源相关领域技术变革的相互作用。他拥有慕尼黑工业大学电气工程硕士学位和苏黎世联邦理工学院博士学位。
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引用次数: 0
Electrified inductive heating for sustainable utilization of liquid hydrogenated organics 电感应加热促进液态氢化有机物的可持续利用
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-21 DOI: 10.1016/j.joule.2024.05.020
Dong Gwon Kang, Kiheon Sung, Hyungseok Yong, Kwanyong Jeong, Myungho Choi, Hyun-Tak Kim, Sunil Kwon, Soo Min Kim, Jin Suk Myung, Dae Woo Kim, Ji Hoon Park, Jeong Woo Han, Sang-Joon Kim

We propose the electrified catalytic inductive heating system (ECIHS), which utilizes electromagnetic induction heating (IH) of a monolithic catalytic composite to induce direct and efficient heat transfer to the liquid-phase reaction environment. Herein, we demonstrated that the ECIHS could be utilized to extract hydrogen from liquid-phase perhydro-dibenzyltoluene (H18-DBT) within just 3.5 s, accounting for a 16.4-fold improvement in the reaction rate compared with conventional heating methods. This remarkable observation underscores the potential of the ECIHS for on-site hydrogen utilization, empowering various advanced applications such as hydrogen-powered vehicles. Furthermore, the capabilities of the ECIHS for efficient heat and mass transfer in the liquid phase are also translatable to a myriad of different chemical processing schemes with high industrial value. Overall, the ECIHS represents a major breakthrough in the development of sustainable chemical processing methods, further propelling efforts to achieve full decarbonization in the global chemical processing industry.

我们提出了电气化催化感应加热系统(ECIHS),该系统利用电磁感应加热(IH)整体催化复合材料,将热量直接有效地传递到液相反应环境中。在这里,我们证明了 ECIHS 可用于在短短 3.5 秒内从液相全氢二苄甲苯(H18-DBT)中提取氢气,与传统加热方法相比,反应速率提高了 16.4 倍。这一引人注目的观察结果凸显了 ECIHS 在现场氢气利用方面的潜力,为氢动力汽车等各种先进应用提供了动力。此外,ECIHS 在液相中高效传热和传质的能力还可应用于各种不同的化学处理方案,具有极高的工业价值。总之,ECIHS 代表着可持续化学处理方法开发方面的重大突破,进一步推动了全球化学处理行业实现全面脱碳的努力。
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引用次数: 0
A data-driven bifunctional oxygen electrocatalyst with a record-breaking ΔE = 0.57 V for ampere-hour-scale zinc-air batteries 一种数据驱动的双功能氧电催化剂,其用于安培小时级锌-空气电池的 ΔE = 0.57 V 值打破了记录
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.03.017
Jia-Ning Liu , Chang-Xin Zhao , Juan Wang , Xuan-Qi Fang , Chen-Xi Bi , Bo-Quan Li , Qiang Zhang

Refreshing the record of the electrocatalytic activity for bifunctional oxygen electrocatalysis is the first priority of developing next-generation rechargeable zinc-air batteries. A ΔE indicator to evaluate the bifunctional electrocatalytic activity has stagnated with a record of ΔE > 0.60 V for decades. Herein, a bifunctional oxygen electrocatalyst is developed to afford an ultrahigh bifunctional electrocatalytic activity of ΔE = 0.57 V and realize high-performance rechargeable zinc-air batteries. Specifically, atomically dispersed Fe-N-C sites and NiFeCe layered double hydroxides are integrated to afford a composite FeNC@LDH electrocatalyst, following the guidance of the data-driven analysis. The FeNC@LDH electrocatalyst demonstrates a record-breaking electrocatalytic activity of ΔE = 0.57 V, far exceeding the state-of-the-art level by ca. 60 mV. Practical ampere-hour-scale zinc-air batteries are constructed with a capacity of 6.4 Ah and cycle under 1.0 A and 1.0 Ah conditions. This work affords a record-breaking bifunctional electrocatalyst for ampere-hour-scale zinc-air batteries in future application scenarios.

刷新双功能氧电催化的电催化活性记录是开发下一代可充电锌-空气电池的首要任务。几十年来,评价双功能电催化活性的 ΔE 指标一直停滞在 ΔE > 0.60 V。在此,我们开发了一种双功能氧电催化剂,使其具有ΔE = 0.57 V 的超高双功能电催化活性,并实现了高性能可充电锌-空气电池。具体来说,在数据驱动分析的指导下,将原子分散的Fe-N-C位点和NiFeCe层状双氢氧化物整合在一起,形成了FeNC@LDH复合电催化剂。FeNC@LDH 电催化剂的电催化活性达到了破纪录的 ΔE = 0.57 V,远远超出最先进水平约 60 mV。我们建造了实用的安培小时锌-空气电池,容量为 6.4 Ah,可在 1.0 A 和 1.0 Ah 的条件下循环使用。这项研究为未来应用场景中的安培小时级锌-空气电池提供了创纪录的双功能电催化剂。
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引用次数: 0
Requirements for CO2-free hydrogen production at scale 大规模无二氧化碳制氢的要求
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.05.010
Eddie Sun , Amitava Sarkar , Marco Gigantino , Richard Randall , Shaffiq Jaffer , Jimmy Rojas , Shang Zhai , Arun Majumdar

Amitava Sarkar is a corporate research scientist for North America at TotalEnergies and a resident visiting scientist at Stanford University working to develop disruptive, no/low-carbon sustainable technologies to decarbonize the chemical industry. He is active in TotalEnergies’ open innovation effort through research and development collaborations and strategic partnerships with various research institutions around the world.

Shaffiq Jaffer is the vice president of corporate science and technology projects in North America at TotalEnergies. He is engaged across the research ecosystem with relationships and investments in academia, startups, and private research companies for the purpose of bringing value to TotalEnergies and its partners.

Arun Majumdar is the inaugural dean of the Stanford Doerr School of Sustainability, the Jay Precourt provostial chair professor at Stanford University, a faculty in the Department of Mechanical Engineering, and a senior fellow and former director of the Stanford Precourt Institute for Energy. He served in the Obama administration as the founding director of the US Department of Energy’s Advanced Research Projects Agency-Energy (ARPA-E) (2009–2012), the acting undersecretary for energy (2011–2012), and as the vice chair of the secretary of energy advisory board (2014–2017). Dr. Majumdar is a member of the US National Academy of Sciences, US National Academy of Engineering, and the American Academy of Arts and Sciences.

Eddie Sun, Marco Gigantino, Richard Randall, Jimmy Rojas, and Shang Zhai were PhD students/postdoctoral scholars at Stanford University at the time of writing. Jimmy Rojas is now the founder and chief executive officer at EvolOH, and Shang Zhai is now an assistant professor in the Department of Mechanical and Aerospace Engineering (with a joint appointment in the School of Earth Sciences) at Ohio State University.

阿米塔瓦-萨卡(Amitava Sarkar)是道达尔能源公司北美地区的企业研究科学家,也是斯坦福大学的常驻访问科学家,致力于开发颠覆性的无碳/低碳可持续技术,以实现化工行业的脱碳。他通过与全球各研究机构的研发合作和战略伙伴关系,积极参与道达尔能源公司的开放式创新工作。Arun Majumdar 是斯坦福大学多尔可持续发展学院首任院长、斯坦福大学 Jay Precourt 教席教授、机械工程系教师、斯坦福 Precourt 能源研究所高级研究员和前所长。他曾在奥巴马政府担任美国能源部能源高级研究计划局(ARPA-E)创始主任(2009-2012 年)、能源部代理副部长(2011-2012 年)和能源部长顾问委员会副主席(2014-2017 年)。孙赟、马可-吉甘蒂诺、理查德-兰德尔、吉米-罗哈斯和翟翔在撰写本文时是斯坦福大学的博士生/博士后学者。Jimmy Rojas 现为 EvolOH 的创始人兼首席执行官,Shang Zhai 现为俄亥俄州立大学机械与航空航天工程系助理教授(与地球科学学院联合聘任)。
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引用次数: 0
Exploring the capabilities and limitations of large language models in the electric energy sector 探索电力能源行业大型语言模型的能力和局限性
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.05.009
Subir Majumder , Lin Dong , Fatemeh Doudi , Yuting Cai , Chao Tian , Dileep Kalathil , Kevin Ding , Anupam A. Thatte , Na Li , Le Xie

Large language models (LLMs) as ChatBots have drawn remarkable attention thanks to their versatile capability in natural language processing as well as in a wide range of tasks. While there has been great enthusiasm toward adopting such foundational model-based artificial intelligence tools in all sectors possible, the capabilities and limitations of such LLMs in improving the operation of the electric energy sector need to be explored, and this commentary identifies fruitful directions in this regard. Key future research directions include data collection systems for fine-tuning LLMs, embedding power system-specific tools in the LLMs, and retrieval augmented generation (RAG)-based knowledge pool to improve the quality of LLM responses and LLMs in safety-critical use cases.

作为聊天机器人的大型语言模型(LLM)因其在自然语言处理和各种任务中的多功能性而备受关注。虽然各行各业都对采用这种基于基础模型的人工智能工具抱有极大的热情,但在改善电力能源行业的运行方面,这种 LLM 的能力和局限性仍有待探索,本评论指出了这方面富有成效的方向。未来的主要研究方向包括用于微调 LLM 的数据收集系统、在 LLM 中嵌入电力系统专用工具,以及基于检索增强生成(RAG)的知识库,以提高 LLM 响应和安全关键用例中 LLM 的质量。
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引用次数: 0
Realizing high-energy and long-life Li/SPAN batteries 实现高能量、长寿命的锂/SPAN 电池
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.04.003
An L. Phan , Phung M.L. Le , Chunsheng Wang

Sulfurized polyacrylonitrile (SPAN) is emerging as a promising cathode for high-energy Li metal batteries. The transition-metal-free nature, high capacity, good sustainability, and low cost serve as competitive advantages of SPAN over conventional layered-oxide counterparts. The unique structure of SPAN with abundant covalent C–S and N–S bonds enables it to achieve high electrochemical performance even in lean electrolyte conditions. Despite great research progress, the current performance of Li/SPAN batteries still falls far behind its true potential. Here, we thoroughly analyze the energy density and cycle life of practical Li/SPAN cells based on our in-house-developed models. Besides, using Sand’s equation, we derive the requirements for Li/SPAN cells to achieve a reasonable power density and discuss their implications. Our analyses address critical issues of Li/SPAN on both material and cell levels, with an emphasis on particularly crucial details that are often overlooked or misunderstood. Accordingly, the challenges and directions for future Li/SPAN research are indicated.

硫化聚丙烯腈(SPAN)正在成为高能锂金属电池的一种前景广阔的阴极。与传统的层状氧化物相比,SPAN 具有不含过渡金属、容量高、可持续性好和成本低等竞争优势。SPAN 结构独特,具有丰富的共价 C-S 和 N-S 键,因此即使在贫电解质条件下也能实现较高的电化学性能。尽管取得了巨大的研究进展,但目前锂/SPAN 电池的性能仍然远远落后于其真正的潜力。在此,我们基于自主开发的模型,全面分析了实用锂/SPAN 电池的能量密度和循环寿命。此外,我们还利用桑德方程推导出锂离子/SPAN 电池达到合理功率密度的要求,并讨论了其影响。我们的分析从材料和电池两个层面探讨了锂/SPAN 电池的关键问题,重点是那些经常被忽视或误解的关键细节。因此,我们指出了未来锂/SPAN 研究的挑战和方向。
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引用次数: 0
High-entropy thermoelectric materials 高熵热电材料
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.04.012
Qiqi Tang , Binbin Jiang , Keli Wang , Wu Wang , Baohai Jia , Tianpeng Ding , Zhenlong Huang , Yuan Lin , Jiaqing He

More than 60% of the energy in the world is wasted during the energy conversion processes but can be potentially collected by thermoelectric (TE) technology. Recently, entropy engineering has been applied in the TE community, yielding numerous high-entropy material systems that exhibit outstanding TE performance. This review outlines the design principles for entropy-stabilized TE materials. Subsequently, it discusses the impact of high entropy on electrical and thermal transport properties. Furthermore, the research advancements of various high-entropy TE material systems are summarized, encompassing IV–VI compounds, half-Heusler (HH) compounds, liquid-like materials, oxide-based ceramics, and other relevant systems. Finally, the conclusion and outlook for high-entropy TE materials are elucidated. Only small regions of high-entropy TE materials have been investigated so far, and there will be vast space that remains to be explored. High-entropy TE materials will be one of the core strategies in the TE community if the optimization mechanism is completely understood.

世界上超过 60% 的能量在能量转换过程中被浪费掉了,但热电(TE)技术却有可能将其收集起来。最近,熵工程已被应用于热电技术领域,产生了许多表现出卓越热电技术性能的高熵材料系统。本综述概述了熵稳定 TE 材料的设计原则。随后,它讨论了高熵对电气和热传输特性的影响。此外,还总结了各种高熵 TE 材料系统的研究进展,包括 IV-VI 化合物、半休斯勒 (HH) 化合物、类液态材料、氧化物基陶瓷和其他相关系统。最后,阐明了高熵 TE 材料的结论和前景。迄今为止,人们只研究了高熵 TE 材料的一小部分,还有广阔的空间有待探索。如果能完全理解优化机制,高熵 TE 材料将成为 TE 界的核心战略之一。
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引用次数: 0
Unveiling transport mechanisms of cesium and water in operando zero-gap CO2 electrolyzers 揭示零间隙二氧化碳电解槽中铯和水的传输机制
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.02.027
Bjørt Óladóttir Joensen , José A. Zamora Zeledón , Lena Trotochaud , Andrea Sartori , Marta Mirolo , Asger Barkholt Moss , Sahil Garg , Ib Chorkendorff , Jakub Drnec , Brian Seger , Qiucheng Xu

In zero-gap CO2 electrolyzers, maintaining the balance of water and cations is crucial. Excessive accumulation at the cathode causes performance degradation, leading to flooding and salt precipitation. Using operando wide-angle X-ray scattering and X-ray fluorescence techniques, we observed the dynamic evolution of H2O and Cs+ inside a membrane electrode assembly. Our findings indicate that Cs+ movement across the membrane from the anode to the cathode is governed by migration and drags H2O via electroosmosis. H2O diffusion then allows Cs+ diffusion further within the gas diffusion electrode. When decreasing the applied voltage, the concentration gradient causes Cs+ to quickly diffuse back to the anode. The H2O content in the macro-porous layer remains at the same level, thus showcasing an origin of gas diffusion electrode (GDE) flooding. By regulating the electrolyte concentration, we deconvolute the correlation of water and cations for selectivity changes. Our work underscores the significance of water/cation management strategies in zero-gap electrolyzers.

在零间隙一氧化碳电解槽中,保持水和阳离子的平衡至关重要。阴极的过度积累会导致性能下降,造成水浸和盐沉淀。我们利用广角 X 射线散射和 X 射线荧光技术,观察了膜电极组件内 HO 和 Cs 的动态演变。我们的研究结果表明,Cs 在膜上从阳极向阴极的移动受迁移的支配,并通过电渗作用拖动 HO。然后,HO 扩散允许 Cs 在气体扩散电极内进一步扩散。当降低外加电压时,浓度梯度会使 Cs 迅速扩散回阳极。大孔层中的 HO 含量保持不变,从而显示了气体扩散电极(GDE)泛滥的起源。通过调节电解质浓度,我们解除了水和阳离子对选择性变化的相关性。我们的工作强调了零间隙电解槽中水/阳离子管理策略的重要性。
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引用次数: 0
Phosphorus-induced anti-growth of ruthenium clusters-single atoms for ultra-stable hydrogen evolution over 100,000 cycles 磷诱导的钌簇反生长--单原子超稳定氢进化超过 100,000 次循环
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.03.005
Zian Xu , Jian Zhu , Zheng Shu , Yu Xia , Rouxi Chen , Shaoqing Chen , Yu Wang , Lin Zeng , Jiacheng Wang , Yongqing Cai , Shi Chen , Fuqiang Huang , Hsing-Lin Wang

Metal aggregation, caused by high current density or long-cycling catalysis, severely affects the stability of ruthenium (Ru)-based catalysts toward hydrogen evolution reaction (HER). Herein, we constructed an anti-growth strategy of phosphorus (P)-induced Ru clusters (1.3 nm) integrated with adjacent Ru single atoms on nitrogen (N)-doped carbon fibers (RuSA/NP-PNCFs) for ultra-stable HER. The RuSA/NP-PNCFs exhibit outstanding activity (8 and 132 mV at 10 and 1,000 mA cm−2) and record durability (100,000 cycles and 1,000 h at 600 mA cm−2). Thanks to the optimized binding energy and orbital interaction between Ru and P/N, the size variation is only 0.8 nm, and single atoms are also well preserved. Both experiments and theoretical simulations indicate that the heteroatom P can not only boost the capacity of H2O dissociation but also suppress the aggregation of Ru clusters and single atoms during HER. This work provides an effective strategy for designing stable metal cluster-single-atom systems for advanced electrocatalysts.

高电流密度或长周期催化导致的金属聚集严重影响了基于钌(Ru)的催化剂在氢进化反应(HER)中的稳定性。在此,我们构建了一种磷(P)诱导的 Ru 簇(1.3 nm)与掺杂氮(N)的碳纤维上的相邻 Ru 单原子集成的抗生长策略(RuSA/NP-PNCFs),用于超稳定 HER。RuSA/NP-PNCFs 具有出色的活性(10 mA cm-2 和 1,000 mA cm-2 时分别为 8 mV 和 132 mV)和创纪录的耐久性(600 mA cm-2 时分别为 100,000 次循环和 1,000 小时)。由于 Ru 和 P/N 之间的结合能和轨道相互作用得到了优化,其尺寸变化仅为 0.8 纳米,而且单原子也得到了很好的保留。实验和理论模拟都表明,杂原子 P 不仅能提高 H2O 的解离能力,还能抑制 HER 过程中 Ru 簇和单个原子的聚集。这项工作为设计用于先进电催化剂的稳定金属团簇-单原子体系提供了有效的策略。
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引用次数: 0
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