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Engineering direct 3d–4f orbital coupling by confining Cu–Ln pairs in paddlewheel metal–organic frameworks for efficient CO electromethanation 通过将Cu-Ln对限制在桨轮金属-有机框架中,设计直接3d-4f轨道耦合,以实现高效的CO电甲烷化
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-19 DOI: 10.1039/d6ee03312a
Guikai Zhang,Ruqi Wang,Can Li,Jiajing Pei,Yue Yu,Yanqiong Zhuang,Zihao Sun,Junpeng Zhu,Ping Wang,Shengqi Chu,Pengfei An,Yuanjun Chen,Juncai Dong
{"title":"Engineering direct 3d–4f orbital coupling by confining Cu–Ln pairs in paddlewheel metal–organic frameworks for efficient CO electromethanation","authors":"Guikai Zhang,Ruqi Wang,Can Li,Jiajing Pei,Yue Yu,Yanqiong Zhuang,Zihao Sun,Junpeng Zhu,Ping Wang,Shengqi Chu,Pengfei An,Yuanjun Chen,Juncai Dong","doi":"10.1039/d6ee03312a","DOIUrl":"https://doi.org/10.1039/d6ee03312a","url":null,"abstract":"Orbital coupling between two ligand-mediated homo-/hetero-metallic species (e.g., d-L-d/s/p) represents a well-established strategy for engineering dual-site catalysts (DSCs). However, its potential to steer complex chemical reactions has not yet been fully unleashed due to the absence of direct metal–metal interaction. Herein, we theoretically predicted that the confinement of copper–lanthanide pairs in a paddlewheel motif exceptionally generates direct 3d–4f orbital coupling via novel σ- and π-bonding, significantly enhancing the adsorption of key intermediates (*CO and *CHO) and thereby indicating facile CO2 electromethanation. Accordingly, we confined a Cu–Er pair within well-defined paddlewheel metal–organic frameworks, where it exhibited definitive 3d–4f orbital coupling. Under a mild potential of −1.1 V vs. RHE, the resulting catalyst reached a superior CH4 faradaic efficiency (FE) of 82% with a partial current density of −251.9 mA cm−2 and a cathode energy efficiency (CEE) of 37.3%, far surpassing the conventional Cu–Cu pair with 31% FECH4 and 14.1% CEE. Moreover, the Cu–Er pair achieved a 2130% increase in CO2-to-CH4 turnover frequency compared to the Cu–Cu pair. Mechanistic studies revealed that direct 3d–4f coupling uniquely accelerates π-backdonation kinetics while stabilizing σ-radical thermodynamics for the *CO hydrogenation to *CHO. Our findings pioneer a transformative approach to designing efficient DSCs through direct d–f coupling under tailored spatial confinement for efficient electrocatalysis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"13 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Simulation of the Electrochemical Reduction of CO 2 to CO from a Bicarbonate Solution 从碳酸氢盐溶液中电化学还原co2为CO的模拟
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-19 DOI: 10.1039/d6ee03258c
Junbo Fu,Adam Z Weber,Clayton J Radke,Alexis T. Bell
{"title":"Simulation of the Electrochemical Reduction of CO 2 to CO from a Bicarbonate Solution","authors":"Junbo Fu,Adam Z Weber,Clayton J Radke,Alexis T. Bell","doi":"10.1039/d6ee03258c","DOIUrl":"https://doi.org/10.1039/d6ee03258c","url":null,"abstract":"CO and synthesis gas can be produced in an energy efficient manner from CO2 absorbed in KOH as KHCO3 using a membrane-electrode assembly (MEA) comprising a Pt anode, a Nafion membrane, and an Ag cathode (an HOR|CEM|HCO3-). We report the development and validation of a one-dimensional multiphysics, continuum model and its use to evaluate engineering modifications needed to achieve economically competitive costs for producing CO and synthesis gas.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"38 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853574","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Buried-Junction Reinforcement through Dual-Sided Interfacial Anchoring in Inverted Perovskite Solar Cells 倒置钙钛矿太阳能电池中双面界面锚定的埋结加固
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-19 DOI: 10.1039/d6ee04307k
Kun Zhang,Xiwen Zhang,Jinxu Wen,Yaning Li,Yang Wang,Haodan Guo,Yongrui Yang,Yu Chen,Yanlin Song
{"title":"Buried-Junction Reinforcement through Dual-Sided Interfacial Anchoring in Inverted Perovskite Solar Cells","authors":"Kun Zhang,Xiwen Zhang,Jinxu Wen,Yaning Li,Yang Wang,Haodan Guo,Yongrui Yang,Yu Chen,Yanlin Song","doi":"10.1039/d6ee04307k","DOIUrl":"https://doi.org/10.1039/d6ee04307k","url":null,"abstract":"Buried interfacial delamination is a major cause of the poor operational stability of inverted perovskite solar cells (PSCs). While, conventional self-assembled monolayers mainly optimize energy-level alignment and fail to establish sufficiently strong coupling across the transparent conductive oxide (TCO)/SAM/perovskite junction. Here, we introduce 2-methyl-4Hthieno[3,2-b]-pyrrole-5-carboxylic acid (MTPCA) as a dual-sided interfacial anchoring molecule to reconstruct the buried contact. MTPCA simultaneously stabilizes SAM anchoring on TCO and strengthens coupling to the perovskite, thereby favor a more robust chemicalmechanical-electronic junction. This reinforced buried interface enhances adhesion strength, promotes more coherent bottom-up crystallization, suppresses interfacial defect accumulation and non-radiative recombination, and improves charge collection under operation-relevant stress. Consequently, the treated devices achieve a champion power conversion efficiency of 27.29% and markedly enhanced operational stability, retaining ~93% of their initial efficiency after nearly 2000 h under ISOS-L-1 and ~90% after 1000 h under ISOS-L-3. Moreover, a representative MTPCA-treated large-area module with an active area of 13.94 cm 2 delivers a power conversion efficiency of 23.69%, supporting the applicability of this buried-junction reinforcement strategy to module-scale device fabrication. This work establishes dual-sided interfacial anchoring as an effective molecular strategy for mitigating buried-interfacial delamination and enabling efficient, mechanically robust, and operationally stable inverted PSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"40 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Redirecting Li-CO₂ Battery Chemistry via Geometric Matching on High-Entropy Intermetallics (110) Facet 高熵金属间化合物几何匹配重定向Li-CO₂电池化学(110)面
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-19 DOI: 10.1039/d6ee04373a
Yang Wang,Qianning Su,Yongjun Li,Xinya Dai,Yiting Liu,Guang Feng,Weifang Liu,Kaiyu Liu,Tao Chen
{"title":"Redirecting Li-CO₂ Battery Chemistry via Geometric Matching on High-Entropy Intermetallics (110) Facet","authors":"Yang Wang,Qianning Su,Yongjun Li,Xinya Dai,Yiting Liu,Guang Feng,Weifang Liu,Kaiyu Liu,Tao Chen","doi":"10.1039/d6ee04373a","DOIUrl":"https://doi.org/10.1039/d6ee04373a","url":null,"abstract":"Steering the Li-CO₂ battery reaction toward the Li₂C₂O₄ pathway is highly appealing yet kinetically hindered by its metastable nature, which renders it prone to disproportionation into Li₂CO₃. Herein, we transcend the conventional d-bandcentric catalytic paradigm by introducing the concept of geometric compatibility factor (δ) as a descriptor for reaction pathway selection. A L1₀-ordered PtZnCoNiFeTi high-entropy intermetallic (PZCNFT-HEI) with crystallographically defined facets is architected to enforce a strain-minimized bridging configuration of Li₂C₂O₄. Atomic-scale interrogations reveal that the (110) facet, counter to the prevalent preference for high-index facets in bond-activation-dominated catalysis, exhibits exceptional δ (97.56%) arising from precise registry between surface dM-M and molecular dO-O. This geometric fidelity engenders a nearly strain-free adsorption geometry, amplifies electronic coupling at the catalyst-intermediate interface, and thermodynamically locks the Li₂C₂O₄ pathway by elevating the kinetic barrier toward its disproportional decomposition.Multimodal characterizations confirm that amorphous Li₂C₂O₄ is preferentially and reversibly formed exclusively on the PZCNFT-HEI cathode. Theoretical analyses reveal that the (110) facet maximizes integrated crystal orbital Hamiltonian population (ICOHP) for Li₂C₂O₄ while suppressing transition metal dissolution via entropic stabilization. Consequently, the assembled Li-CO₂ battery achieves a high discharge voltage of 3.11 V and stable operation over 200 cycles. This work establishes geometric compatibility factor as a quantitative selection rule for stabilizing metastable intermediates, challenging conventional facet-activity paradigms and opening a non-ergodic design landscape for high-entropy electrocatalysts.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"28 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853572","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Molecular-to-system engineering for long-life aqueous zinc-ion batteries for grid-scale energy storage 用于电网级储能的长寿命水性锌离子电池的分子到系统工程
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee02967a
Jihwan Byun,Minkwan Kim,Seung Hyun Jeong,Jang Wook Choi
{"title":"Molecular-to-system engineering for long-life aqueous zinc-ion batteries for grid-scale energy storage","authors":"Jihwan Byun,Minkwan Kim,Seung Hyun Jeong,Jang Wook Choi","doi":"10.1039/d6ee02967a","DOIUrl":"https://doi.org/10.1039/d6ee02967a","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) are promising candidates for grid-scale energy storage. However, zinc corrosion during non-operational periods accelerates calendar aging and undermines their long-term operability, particularly under realistic operating conditions with idle intermittency. Herein, we present a molecular-to-system-level strategy to suppress corrosive degradation and enhance lifetime-delivered energy. At the molecular level, the diethyl [difluoro(trimethylsilyl)methyl]phosphonate (DEDFTMSP) co-solvent extensively dehydrates the Zn2+ solvation structure and promotes ion-pair states that drive the formation of an inorganic, corrosion-resistant interphase, while the hexamethylphosphoramide (HMPA) additive shields interphasial defects on the Zn surface. At the system level, we propose a sacrificial battery stabilization system (SBSS), wherein a persistent electric field mitigates water-induced corrosion through the accumulation of charged species in the electric double layer with minimal energy cost. The combined strategy delivers markedly improved capacity retention and total discharged energy under practically relevant conditions, establishing a comprehensive approach toward durable, resource-efficient solutions for grid-scale energy storage.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"49 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148767747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Deep eutectic solvents for high-efficiency and short-process recycling of spent lithium-ion batteries: progress, challenges, and perspectives 深共晶溶剂用于废旧锂离子电池的高效短流程回收:进展、挑战和展望
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee02671k
Xiaoyu Liu,Zhili Tang,Xu Liu,Siqi Long,Rui Huang,Yue Wang,Huiyi Tian,Jing Tan,Kunpeng Li,Xu Yan,Haiying Wang,Xiaobo Min,Jiexi Wang,Fangli Zhang,Zaiping Guo,Wenchao Zhang,Liyuan Chai
{"title":"Deep eutectic solvents for high-efficiency and short-process recycling of spent lithium-ion batteries: progress, challenges, and perspectives","authors":"Xiaoyu Liu,Zhili Tang,Xu Liu,Siqi Long,Rui Huang,Yue Wang,Huiyi Tian,Jing Tan,Kunpeng Li,Xu Yan,Haiying Wang,Xiaobo Min,Jiexi Wang,Fangli Zhang,Zaiping Guo,Wenchao Zhang,Liyuan Chai","doi":"10.1039/d6ee02671k","DOIUrl":"https://doi.org/10.1039/d6ee02671k","url":null,"abstract":"The rapid expansion of the electric vehicle and energy storage sectors has driven unprecedented demand for sustainable recycling of spent lithium-ion batteries (LIBs). Conventional recycling technologies such as pyrometallurgy and hydrometallurgy typically suffer from high energy consumption, environmental pollution, and lengthy workflows. Recently, deep eutectic solvents (DESs) have gained considerable attention for resource recovery due to their potential to enable a green, efficient, and short-process recycling route. Nevertheless, the practical application of DESs still faces considerable scepticism, owing to their dependence on high temperatures, low solid-to-liquid (S/L) ratios, and high costs. In this review, we focus on the intrinsic properties of DESs and the key mechanisms governing their role in metal recovery and material regeneration. Building on this, we provide perspectives on future development spanning DES design, characterization techniques, expansion application, techno-economic and environmental assessment, policy incentives and industrial compatibility. These insights aim to clarify the current trends in the application and development of DESs for spent battery recycling, while identifying future directions for their practical utilization.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"37 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148767793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Synergy of extended exciton transport and strong exciton–CT state coupling in NIR organic photocatalysts 近红外有机光催化剂中扩展激子输运和强激子- ct态耦合的协同作用
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee03349k
Yunzhi Wang,Partha Maity,Simil Thomas,Lingyun Zhao,Yanru Li,Lijie Wang,Zhuping Fei,Niveen M. Khashab,Omar F. Mohammed,Huabin Zhang
{"title":"Synergy of extended exciton transport and strong exciton–CT state coupling in NIR organic photocatalysts","authors":"Yunzhi Wang,Partha Maity,Simil Thomas,Lingyun Zhao,Yanru Li,Lijie Wang,Zhuping Fei,Niveen M. Khashab,Omar F. Mohammed,Huabin Zhang","doi":"10.1039/d6ee03349k","DOIUrl":"https://doi.org/10.1039/d6ee03349k","url":null,"abstract":"Organic semiconductor (OSC) photocatalysts often suffer from inefficient free charge generation due to the limited exciton diffusion length (LD), particularly in narrow-bandgap OSCs that harvest near-infrared (NIR) light. Here, we report blend nanoparticles (NPs) composed of the donor polymer PFBDB-T and the non-fused acceptor BTOR-IC4F, which achieve markedly enhanced hydrogen (H2) evolution through the synergistic effect of extended exciton transport and strong exciton–charge transfer (CT) state coupling. In particular, the H2 evolution reaction rate of PFBDB-T:BTOR-IC4F heterojunction NPs with photodeposited Pt is 27-fold higher than that of platinum (Pt)-loaded PFBDB-T NPs and an order of magnitude higher than that of Pt-loaded BTOR-IC4F NPs under visible–near-infrared (Vis-NIR) light illumination. Transient absorption spectroscopy reveals the generation of long-lived free carriers (2.85 ns) even when NIR photons serve as the sole energy input. Decay dynamics analysis demonstrates the significantly extended exciton diffusion length (17.1 nm) in PFBDB-T:BTOR-IC4F NPs relative to that in pristine single-component NPs, while time-dependent density functional theory calculations elucidate the strong exciton–charge transfer (CT) state coupling (66.7 meV) in the PFBDB-T:BTOR-IC4F blend. The elongated exciton diffusion contributes to the strong exciton–CT state coupling, which in turn prolongs the exciton transport. These findings highlight a general strategy to improve NIR-driven photocatalysis in organic heterojunction systems by leveraging the synergistic effect of extended exciton transport and strong exciton–CT state interaction.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"33 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148767743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Unveiling the Hidden Junction: Metrology of Buried Perovskite/SAM Interfaces for High-Efficiency Solar Cells 揭示隐藏结:高效太阳能电池中埋藏钙钛矿/SAM界面的计量学
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee03893j
Jianhua Zhou,Yuliang Che,Zhuoer Cai,Ariany Bonadio,Zhiqun Lin,Shuzhi Liu
{"title":"Unveiling the Hidden Junction: Metrology of Buried Perovskite/SAM Interfaces for High-Efficiency Solar Cells","authors":"Jianhua Zhou,Yuliang Che,Zhuoer Cai,Ariany Bonadio,Zhiqun Lin,Shuzhi Liu","doi":"10.1039/d6ee03893j","DOIUrl":"https://doi.org/10.1039/d6ee03893j","url":null,"abstract":"Strategic engineering of the buried interface between self-assembled monolayers (SAMs) and perovskites has propelled the certified efficiency of perovskite solar cells (PSCs) beyond 27%. Nevertheless, the intrinsically inaccessible nature of this hidden junction poses a formidable metrological challenge, hindering the comprehensive characterization required to guide future performance breakthroughs. This review systematically examines current approaches for probing the perovskite/SAM interface, spanning destructive ex situ techniques that risk introducing mechanical artifacts, and non-destructive indirect probes, often hindered by signal interference from underlying functional layers. While emerging high-penetration tools such as hard X-ray photoelectron spectroscopy (HAXPES) and neutron reflectometry (NR) offer complementary depth-sensitive access to buried interfaces, a metrological gap persists between idealized thin-film samples and realistic device architectures. We further present perspectives encompassing advanced sample preparation protocols, rational substrate engineering, deeper penetration techniques advocate, multimodal operando measurement methodologies and AI-assisted data processing. By outlining key challenges and opportunities in buried interface metrology, this review aims to guide future developments and accelerate the advancement and commercialization of PSC technologies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"20 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148853565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Identification and understanding of activation procedures critical for nickel-based anodes in anion-exchange membrane fuel cells 阴离子交换膜燃料电池中镍基阳极关键活化过程的识别和理解
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee03112a
Simon Amigues,Nicolas Bibent,Eliot Petitdemange,Estelle Guyennot,Frédéric Lecoeur,Marc Dupont,Meryem Ennaji,Amir Gasmi,Raphaël Chattot,Michal Ronovsky,Laetitia Dubau,Frédéric Maillard,Jakub Drnec,Tomáš Hrbek,Patrick Elsaesser,Sima Heidari,Anna Fischer,Liela Clarke,Xinqi Chen,Ahmed A. Farghaly,Syeda Mushrifa Zahan,Alexander A. Baranov,Dario R. Dekel,Frédéric Jaouen
{"title":"Identification and understanding of activation procedures critical for nickel-based anodes in anion-exchange membrane fuel cells","authors":"Simon Amigues,Nicolas Bibent,Eliot Petitdemange,Estelle Guyennot,Frédéric Lecoeur,Marc Dupont,Meryem Ennaji,Amir Gasmi,Raphaël Chattot,Michal Ronovsky,Laetitia Dubau,Frédéric Maillard,Jakub Drnec,Tomáš Hrbek,Patrick Elsaesser,Sima Heidari,Anna Fischer,Liela Clarke,Xinqi Chen,Ahmed A. Farghaly,Syeda Mushrifa Zahan,Alexander A. Baranov,Dario R. Dekel,Frédéric Jaouen","doi":"10.1039/d6ee03112a","DOIUrl":"https://doi.org/10.1039/d6ee03112a","url":null,"abstract":"Anion-exchange membrane fuel cells (AEMFCs) hold promise as high-performance devices free of platinum group metals. A major bottleneck to achieve this goal is the moderate performance of nickel-based anodes. Metallic nickel is critical for hydrogen binding, which is essential for the electrocatalysis of the hydrogen oxidation reaction (HOR), but is prone to passivation. Here, we show that for representative mainstream Ni-based catalysts, their spontaneous passivation in ambient air blocks the HOR, necessitating activation protocols. In a three-electrode rotating-disk electrode setup, activation is readily accomplished by lowering the electrode potential. In an AEMFC, galvanostatic and chemical activation strategies are explored, revealing the strong influence of O2 crossover from the cathode, which can repassivate Ni. Chemical activation involving an initial H2/N2 feed at the anode/cathode proved to be the most practical, enabling a high open-circuit voltage, power density and stability in subsequent H2/O2 and H2/air AEMFC measurements. A chemically activated Ni@NC anode paired with a Pt/C cathode achieved an outstanding AEMFC peak power density of 1.2 W cm−2 using H2/O2 as feed and an unprecedented peak power density of 0.5 W cm−2 using H2/air (ambient) as feed.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"37 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148767745","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Unlocking longevity of anode-free lithium batteries: the role of mass transport 解锁无阳极锂电池的寿命:大规模运输的作用
IF 32.5 1区 材料科学
Energy & Environmental Science Pub Date : 2026-08-18 DOI: 10.1039/d6ee01541g
Yi He,Saeed Habibpour,Hey Woong Park,Qiran Lu,Shuxuan Mao,Elena Bekyarova,Aiping Yu
{"title":"Unlocking longevity of anode-free lithium batteries: the role of mass transport","authors":"Yi He,Saeed Habibpour,Hey Woong Park,Qiran Lu,Shuxuan Mao,Elena Bekyarova,Aiping Yu","doi":"10.1039/d6ee01541g","DOIUrl":"https://doi.org/10.1039/d6ee01541g","url":null,"abstract":"Mass transport plays a pivotal role in the electrochemical processes of anode-free lithium metal batteries (AFLMBs), where the absence of an excess lithium reservoir imposes strict requirements on lithium-ion transfer during cycling. Effective regulation of mass transport behaviors—such as ion flux distribution and transport kinetics—can significantly influence local concentration gradients, suppress dendrite growth, and control lithium deposition morphology. These mass transport improvements are essential to enhancing coulombic efficiency, prolonging cycle life, and ensuring stability of AFLMBs. This review comprehensively summarizes progress in AFLMBs from the perspective of mass transport regulation. We begin by outlining the fundamental principles of Li+ transport in anode-free configurations and elucidating its pivotal role in governing lithium plating/stripping behavior and the retention of active lithium. Subsequently, we highlight advances in electrolyte engineering, current collector modification, mechanical confinement, thermal environment optimization, and pre-lithiation strategies, each tailored to modulate ion flux and improve interfacial stability. Particular emphasis is placed on how these regulatory approaches synergistically promote uniform lithium nucleation and enhance cycling reversibility. Lastly, we outline future directions to guide the rational design of mass-transport pathways, thereby enhancing interfacial stability and unlocking the intrinsic energy storage potential of AFLMBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148767818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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