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Toward photovalorization of waste at scale? 实现大规模废物光氧化?
IF 38.6 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1016/j.joule.2024.06.021

The identification of green strategies for ammonia production is critical, and nitrate reduction has emerged as a promising approach. In a recent issue of Nature Catalysis, Tayyebi et al. reported unprecedented ammonia production rates via bias-free photochemical nitrate reduction coupled with glycerol oxidation.

确定氨生产的绿色战略至关重要,而硝酸盐还原已成为一种很有前景的方法。Tayyebi 等人在最近一期的《自然催化》(Nature Catalysis)杂志上报告了通过无偏差光化学硝酸盐还原与甘油氧化耦合产生氨的前所未有的生产率。
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引用次数: 0
Strained heterojunction enables high-performance, fully textured perovskite/silicon tandem solar cells 应变异质结实现了高性能、完全纹理化的过氧化物/硅串联太阳能电池
IF 39.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1016/j.joule.2024.06.015

Integrating metal-halide perovskites with the industrially textured Czochralski silicon for perovskite/silicon tandem cells shows great promise for low-cost manufacturing and ideal light trapping. However, the conformal growth of high-quality perovskite film on fully textured silicon remains challenging due to the lack of effective regulation of structural evolution and residual strains. Here, we report a strain regulation strategy by forming a 3D/3D perovskite heterojunction at the buried interface through a vacuum-deposition method applicable to pyramidal texture. By tailoring the composition of buried buffer 3D perovskite, a controllable compressive strain is applied to the upper photoactive 3D perovskite, alleviating its residual tensile stress. We demonstrate that this strained heterostructure promotes the preferred crystal growth, reduces interfacial defect-induced recombination, and facilitates charge extraction. As a result, the fully textured perovskite/silicon tandem cell achieves a certified steady-state efficiency of 31.5% and retains over 95% of its initial efficiency after 800 h of continuous operation.

将金属卤化物包晶石与工业化纹理 Czochralski 硅整合在一起,制成包晶石/硅串联电池,有望实现低成本制造和理想的光捕获。然而,由于缺乏对结构演化和残余应变的有效调节,在完全纹理硅上保形生长高质量的包光体薄膜仍然具有挑战性。在此,我们报告了一种应变调节策略,即通过适用于金字塔纹理的真空沉积方法,在埋藏界面形成三维/三维包晶异质结。通过调整埋藏缓冲三维过氧化物的成分,对上层光活性三维过氧化物施加可控压应变,从而减轻其残余拉应力。我们证明,这种应变异质结构能促进优先晶体生长,减少界面缺陷引起的重组,并有利于电荷提取。因此,完全纹理化的透辉石/硅串联电池实现了 31.5% 的认证稳态效率,并在连续运行 800 小时后保持了 95% 以上的初始效率。
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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
Semi-supervised learning for explainable few-shot battery lifetime prediction 半监督学习用于可解释的少量电池寿命预测
IF 39.8 1区 材料科学 Q1 Energy Pub Date : 2024-06-19 DOI: 10.1016/j.joule.2024.02.020
Nanlin Guo , Sihui Chen , Jun Tao , Yang Liu , Jiayu Wan , Xin Li

Accurate prediction of battery lifetime is critical for ensuring timely maintenance and safety of batteries. Although data-driven methods have made significant progress, their model accuracy is often hampered by a scarcity of labeled data. To address this challenge, we developed a semi-supervised learning technique named partial Bayesian co-training (PBCT), enhancing the modeling of battery lifetime prediction. Leveraging the low-cost unlabeled data, our model extracts hidden information to improve the understanding of the underlying data patterns and achieve higher lifetime prediction accuracy. PBCT outperforms existing approaches by up to 21.9% on lifetime prediction accuracy, with negligible overhead for data acquisition. Moreover, our research suggests that incorporating unlabeled data into the training process can help to uncover critical factors that impact battery lifetime, which may be overlooked with a limited number of labeled data alone. The proposed semi-supervised approach sheds light on the future direction for efficient and explainable data-driven battery status estimation.

准确预测电池寿命对于确保电池的及时维护和安全至关重要。尽管数据驱动方法已取得重大进展,但其模型准确性往往受到标记数据稀缺的影响。为了应对这一挑战,我们开发了一种名为 "部分贝叶斯协同训练"(PBCT)的半监督学习技术,以增强电池寿命预测的建模能力。利用低成本的非标记数据,我们的模型提取了隐藏信息,从而提高了对底层数据模式的理解,实现了更高的寿命预测精度。在寿命预测准确率方面,PBCT 比现有方法高出 21.9%,而数据采集的开销几乎可以忽略不计。此外,我们的研究还表明,将未标记数据纳入训练过程有助于发现影响电池寿命的关键因素,而仅使用有限数量的标记数据可能会忽略这些因素。所提出的半监督方法为高效、可解释的数据驱动型电池状态估算指明了未来的方向。
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引用次数: 0
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Joule
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