ACS Energy Letters 最新文献_第7页

Designing Pitch-Derived Spherical Hard Carbon via Catalytic Aerobic Oxidation and Closed-Pore Regulation 通过催化好氧氧化和闭孔调控设计沥青衍生球形硬碳

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-07 DOI: 10.1021/acsenergylett.6c01910

Shuhui Li, Weihuang Wang, Rui Liu, Zheng Wang, Chenglu Huang, Hongliang Li, Xinxin Cao, Jiang Zhou, Liangbing Wang, Jie Zeng

{"title":"Designing Pitch-Derived Spherical Hard Carbon via Catalytic Aerobic Oxidation and Closed-Pore Regulation","authors":"Shuhui Li, Weihuang Wang, Rui Liu, Zheng Wang, Chenglu Huang, Hongliang Li, Xinxin Cao, Jiang Zhou, Liangbing Wang, Jie Zeng","doi":"10.1021/acsenergylett.6c01910","DOIUrl":"10.1021/acsenergylett.6c01910","url":null,"abstract":"Pitch-derived hard carbon emerges as an anode material for sodium-ion batteries, but its performance still suffers from the trade-offs among plateau capacity, rate capability, and compaction density. Herein, a catalytic aerobic oxidation strategy that enables controllable oxidation of pitch is employed to fabricate spherical hard carbon with tunable pore structures, realizing simultaneous enhancement of these abovementioned metrics. The spherical hard carbon achieves charging of 126.5 mAh g–1 within about 50 s and sustains sodium storage over continuous 1000 cycles at 9 A g–1. Under an increased areal loading, the anode maintains an areal capacity of 1.65 mAh cm–2, a volumetric capacity up to 332.6 mAh cm–3 and endures 100 charge–discharge cycles at a current density of nearly 3 mA cm–2. This work provides a strategy to design hard carbon anodes with enhanced volumetric capacity and rate performance for space-constrained energy storage scenarios.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6669–6679"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973162","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

Stabilizing High-Voltage Operation in O3-Type Na-Layered Cathodes by Suppressing Distortion-Driven Fe Migration 通过抑制扭曲驱动的铁迁移来稳定o3型na层阴极的高压运行

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-09 DOI: 10.1021/acsenergylett.6c02530

Taegyu Kim, Hyunji Kweon, Hoseok Lee, Lahyeon Jang, Bonyoung Ku, Myungeun Choi, Sunghyun Lim, Heejin Choo, Lisa Eom, Junha Kwon, Min-Kyung Cho, Young Hwa Jung, Hun-Gi Jung, Jongsoon Kim

{"title":"Stabilizing High-Voltage Operation in O3-Type Na-Layered Cathodes by Suppressing Distortion-Driven Fe Migration","authors":"Taegyu Kim, Hyunji Kweon, Hoseok Lee, Lahyeon Jang, Bonyoung Ku, Myungeun Choi, Sunghyun Lim, Heejin Choo, Lisa Eom, Junha Kwon, Min-Kyung Cho, Young Hwa Jung, Hun-Gi Jung, Jongsoon Kim","doi":"10.1021/acsenergylett.6c02530","DOIUrl":"10.1021/acsenergylett.6c02530","url":null,"abstract":"Fe-based O3-type Na-layered oxides such as Na[Ni1/3Fe1/3Mn1/3]O2 are attractive cathodes based on earth-abundant elements, yet their high-voltage operation is limited by voltage decay and capacity fading. Here, we identify a distortion−migration cascade initiated by Fe3+ oxidation to Fe4+. The resulting Jahn−Teller distortion of FeO6 octahedra destabilizes Fe within the transition-metal (TM) framework. This destabilization promotes Fe migration into the Na layer and drives irreversible layered to rocksalt-like reconstruction. A stepwise strategy that reduces the Fe content, reinforces the TM−O framework, and blocks Fe migration into the Na layer interrupts this cascade. The optimized cathode delivers 177.96 mAh g−1 with an initial Coulombic efficiency of 94.1% and retains 73.5% capacity after 100 cycles. Experimental and computational analyses reveal continuous structural evolution and suppressed Fe migration. These results establish suppression of distortion-driven Fe migration as a key design principle for stabilizing high-voltage operation in Fe-based Na-layered cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6972–6980"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148933368","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

Dipolar-Steric Cage Diammonium Passivation for Perovskite/Tunnel Oxide Passivated Contact Tandem Solar Cells 钙钛矿/隧道氧化物钝化接触式串联太阳能电池的偶极空间笼型钝化

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-15 DOI: 10.1021/acsenergylett.6c01941

Junxiao He, Bowen Yang, Wenhao Li, Anqi Lv, Shibo Wang, Zijia Li, Weichun Pan, Xianyuan Jiang, Bo Gao, Liu Yang, Kun Gao, Chang Wang, Wei Shi, Fengxian Cao, Li Tan, Xinyao Sun, Gege Yan, Xudong Chen, Zhongliang Yan, Xueying Yang, Yang Bai, Jun Yin, Chenxu He, Xinbo Yang

{"title":"Dipolar-Steric Cage Diammonium Passivation for Perovskite/Tunnel Oxide Passivated Contact Tandem Solar Cells","authors":"Junxiao He, Bowen Yang, Wenhao Li, Anqi Lv, Shibo Wang, Zijia Li, Weichun Pan, Xianyuan Jiang, Bo Gao, Liu Yang, Kun Gao, Chang Wang, Wei Shi, Fengxian Cao, Li Tan, Xinyao Sun, Gege Yan, Xudong Chen, Zhongliang Yan, Xueying Yang, Yang Bai, Jun Yin, Chenxu He, Xinbo Yang","doi":"10.1021/acsenergylett.6c01941","DOIUrl":"10.1021/acsenergylett.6c01941","url":null,"abstract":"Resolving the long-standing trade-off between effective interfacial passivation and efficient charge transport remains a central challenge for perovskite/silicon tandem solar cells, particularly at the perovskite/C60 interface. Here, inspired by the bio-isostere concept, we introduce a dipolar cage strategy that replaces traditional planar phenyl motifs with a rigid bicyclo[2.2.2]octane (BCO) scaffold. Distinct from conventional passivators relying solely on steric shielding, the BCO framework imparts a substantial intrinsic molecular dipole. This architecture establishes a favorable interfacial electrostatic field, substantially reducing the interfacial energetic mismatch for electron extraction while effectively suppressing nonradiative recombination. Utilizing bicyclo[2.2.2]octane-1,4-diammonium diiodide (BCODAI), monolithic perovskite/tunnel oxide passivated contact (TOPCon) tandem solar cells achieve a certified champion efficiency of 32.54%. Crucially, the devices exhibit outstanding operational stability, retaining over 80% of their initial efficiency after 1100 h of continuous operation. This dipolar-steric cage design provides an effective interfacial engineering principle for high-performance tandem photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6697–6706"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973619","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

Phenoxazine or Phenothiazine: From Heteroatom Substitution to Conformational Change and Interfacial Effects of π-Conjugated Ligands in 2D/3D Perovskite Solar Cells 苯恶嗪或吩噻嗪：从杂原子取代到π共轭配体在2D/3D钙钛矿太阳能电池中的构象变化及界面效应

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-26 DOI: 10.1021/acsenergylett.6c00934

Huaiman Cao, Yicong Duan, Xufan Zheng, Liangyu Zhao, Yulong Chen, Zheng Lv, Zhiguang Sun, Yingguo Yang, Hin-Lap Yip, Ze Yu

{"title":"Phenoxazine or Phenothiazine: From Heteroatom Substitution to Conformational Change and Interfacial Effects of π-Conjugated Ligands in 2D/3D Perovskite Solar Cells","authors":"Huaiman Cao, Yicong Duan, Xufan Zheng, Liangyu Zhao, Yulong Chen, Zheng Lv, Zhiguang Sun, Yingguo Yang, Hin-Lap Yip, Ze Yu","doi":"10.1021/acsenergylett.6c00934","DOIUrl":"10.1021/acsenergylett.6c00934","url":null,"abstract":"Utilizing π-conjugated ligands offers opportunities to ameliorate intermolecular interactions between spacer cations, improving charge transport in 2D perovskites. We develop two new ligands by incorporating phenoxazine (PXZ) or phenothiazine (PTZ) moieties, namely PXZEAI and PTZEAI, in which oxygen-to-sulfur substitution induces the intrinsically coupled effects of a more folded conformation (17° smaller dihedral angle) and interfacial chemistry. Unexpectedly, X-ray diffraction (XRD) analysis exhibits distinct lattice spacings in (PTZEA)2PbI4 (16.81 Å) and (PXZEA)2PbI4 (20.36 Å). Density functional theory simulations and synchrotron radiation single-crystal XRD reveal closer packing for (PTZEA)2PbI4, consistent with stronger intermolecular π–π interaction enabled by a more folded conformation, together with sulfur-specific interfacial effects. Grazing incidence wide-angle X-ray scattering results further support π–π interactions between PTZEA+ cations. Ultimately, a contrasting efficiency trend is observed in 2D/3D perovskite solar cells (PTZEAI (25.28%) > control (23.18%) > PXZEAI (19.08%)). This performance difference reflects the synergy of heteroatom-driven conformational change and sulfur-mediated interfacial effects.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6466–6475"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049806","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

Halide Effects on Platinum Co-Catalysts Govern Photocatalytic Hydrogen Evolution in Organic Semiconductor Nanoparticles 卤化物效应对有机半导体纳米粒子光催化析氢的影响

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-29 DOI: 10.1021/acsenergylett.6c01928

Arnau Bertran, Aurélie Célérien, Arthur E. Bouchez, Melanie Johanning, Colin Jeanguenat, Jin Su Park, Jun-Ho Yum, Kevin Sivula

{"title":"Halide Effects on Platinum Co-Catalysts Govern Photocatalytic Hydrogen Evolution in Organic Semiconductor Nanoparticles","authors":"Arnau Bertran, Aurélie Célérien, Arthur E. Bouchez, Melanie Johanning, Colin Jeanguenat, Jin Su Park, Jun-Ho Yum, Kevin Sivula","doi":"10.1021/acsenergylett.6c01928","DOIUrl":"10.1021/acsenergylett.6c01928","url":null,"abstract":"Platinum cocatalysts are essential for photocatalytic hydrogen evolution by organic semiconductor (OSC) bulk-heterojunction nanoparticles (BHJ NPs), yet the surface chemistry of photodeposited Pt remains poorly understood. Here, we show that the halide ligand in hexahaloplatinate(IV) precursors (K2PtX6, X = Cl, Br, I) critically governs both the kinetics of Pt photodeposition and the resulting photocatalytic performance. Chloroplatinate precursors leave partially reduced [PtClx]n species adsorbed on the Pt surface, poisoning active sites and severely suppressing H2 evolution rates in BHJ systems that generate low photopotential, which is confirmed by photoelectrochemical measurements and Kelvin-probe force microscopy. Bromo- and iodoplatinate precursors reduce more readily, largely avoiding this poisoning. Remarkably, the addition of iodide ions to the photocatalytic mixture provides a substantial and general boost to H2 evolution rates, reaching an apparent quantum yield of 17% at 700 nm (among the highest reported for BHJ NP photocatalysts) attributed to beneficial iodide adsorption on the Pt surface.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6690–6696"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090600","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

Dual Strategy of Molecular-Weight Control and Ionic Doping in Poly(benzodifurandione) for Energy-Efficient Neuromorphic Organic Electrochemical Transistors 高效能神经形态有机电化学晶体管中聚苯并二呋喃二酮的分子量控制和离子掺杂双重策略

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-29 DOI: 10.1021/acsenergylett.6c02367

José Carlos Pérez-Martínez, Ignacio Sanjuán, David Franco, Isaac Sánchez-Márquez, Baurzhan Ilyassov, Qun-Gao Chen, Wen-Ya Lee, Chu-Chen Chueh, Antonio Guerrero

{"title":"Dual Strategy of Molecular-Weight Control and Ionic Doping in Poly(benzodifurandione) for Energy-Efficient Neuromorphic Organic Electrochemical Transistors","authors":"José Carlos Pérez-Martínez, Ignacio Sanjuán, David Franco, Isaac Sánchez-Márquez, Baurzhan Ilyassov, Qun-Gao Chen, Wen-Ya Lee, Chu-Chen Chueh, Antonio Guerrero","doi":"10.1021/acsenergylett.6c02367","DOIUrl":"10.1021/acsenergylett.6c02367","url":null,"abstract":"Poly(benzodifurandione) (PBFDO) is a promising n-type mixed conductor for organic electrochemical transistors (OECTs), but its high intrinsic conductivity results in excessive operating currents and energy consumption for neuromorphic computing. Here, we combine molecular-weight engineering and ionic doping to overcome this limitation. Benzofuranone end-capping produces a reduced chain length polymer (PBFDO-BF) with substantially lower intrinsic conductivity, while LiTFSI doping enhances ion-mediated conductance modulation and synaptic functionality. PBFDO-BF + LiTFSI provides enhanced OECT modulation and spike-dependent plasticity while reducing operating currents by approximately 1 order of magnitude compared with pristine PBFDO. In the Modified National Institute of Standards and Technology (MNIST)-based convolutional neural network simulations, the device achieves 97.8% training and 98.6% inference accuracy, with the lowest cumulative energy consumption to reach ≈90% accuracy. These results establish molecular-weight control combined with ionic doping as an effective strategy for developing energy-efficient PBFDO-based neuromorphic OECTs without compromising stability or solution processability.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6940–6949"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091013","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

Enhancing the Interphasic Stability of Sodium-Ion Batteries via Structural Distortion-Driven Defluorination of Aromatic Additives 结构畸变驱动芳香添加剂脱氟提高钠离子电池的相间稳定性

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-02 DOI: 10.1021/acsenergylett.6c01569

Seungwon Jang, Changhoon Park, Wonjun Song, Dongjoon Kim, Dongwoo Kim, Yewon Shin, Hyemi Park, Hee-Tak Kim

{"title":"Enhancing the Interphasic Stability of Sodium-Ion Batteries via Structural Distortion-Driven Defluorination of Aromatic Additives","authors":"Seungwon Jang, Changhoon Park, Wonjun Song, Dongjoon Kim, Dongwoo Kim, Yewon Shin, Hyemi Park, Hee-Tak Kim","doi":"10.1021/acsenergylett.6c01569","DOIUrl":"10.1021/acsenergylett.6c01569","url":null,"abstract":"The commercial viability of sodium-ion batteries is hindered by the interphasic instability of hard carbon (HC) anodes. Here, we reveal a fundamentally new interphasic engineering mechanism driven by the reduction-induced structural distortion of fluorinated aromatic additives (FAAs). We demonstrate that 1,2-difluorobenzene (2FB) preferentially accumulates at the HC interface via strong π–π interactions. Crucially, upon reduction, 2FB undergoes profound structural distortion driven by π* and σ* orbital mixing. This deformation significantly weakens the C–F bond, triggering facile defluorination to construct a robust, sodium fluoride (NaF)-rich inorganic solid electrolyte interphase (SEI). This highly protective, thin layer suppresses continuous SEI dissolution and hazardous Na plating while accelerating Na+ transport kinetics. Consequently, HC || Na(Ni1/3Fe1/3Mn1/3)O2 full cells delivered enhanced cycling stability under 3C fast-charging conditions. This work establishes a molecular design principle for engineering advanced electrochemical interfaces through orbital-level structural manipulation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6516–6524"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148885267","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

Strong Hydrogen Bond Interaction Induced Dimensional Evolution in Aromatic Diammonium-Based Perovskite/Perovskitoid for Achieving High-Performance X-ray Detection 强氢键相互作用诱导芳香族二胺基钙钛矿/类钙钛矿实现高性能x射线探测的尺寸演化

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-10 DOI: 10.1021/acsenergylett.6c01440

Zimin Zhang, Xiaodie Zhang, Huayang Li, Depeng Chu, Le Ye, Yueyao Li, Guangcheng Weng, Lanhua Yi, Yucheng Liu, Shi Chen, Xingzhu Wang

{"title":"Strong Hydrogen Bond Interaction Induced Dimensional Evolution in Aromatic Diammonium-Based Perovskite/Perovskitoid for Achieving High-Performance X-ray Detection","authors":"Zimin Zhang, Xiaodie Zhang, Huayang Li, Depeng Chu, Le Ye, Yueyao Li, Guangcheng Weng, Lanhua Yi, Yucheng Liu, Shi Chen, Xingzhu Wang","doi":"10.1021/acsenergylett.6c01440","DOIUrl":"10.1021/acsenergylett.6c01440","url":null,"abstract":"2D perovskite single crystals (SCs) based on various aromatic diammonium cations have demonstrated significant potential in high-performance X-ray detection. Nevertheless, the relationship between the structure of aromatic diammonium cations and perovskite dimension remains elusive. Herein, four aromatic diamine ligands of 4,4′-bipyridine (BPD), 4,4′-azopyridine (APD), 4,4′-vinylenedipyridine (VPD), and 4,4′-ethylenedipyridine (EPD) are selected to synthesize the target perovskites. A dimensional evolution from non-perovskite (EPDI2)•I2, 1D perovskitoids (BPD)PbI4 and (VPD)Pb2I6 to 2D perovskite (APD)PbI4 is observed. The strong hydrogen bond interactions contribute to edge-to-face arrangement of APD2+ cations instead of face-to-face packing of BPD2+, VPD2+ and EPD2+ cations, efficiently weakening the intermolecular cation–π interaction. Additionally, 2D (APD)PbI4 SCs feature enhanced crystallization quality, lattice rigidity, and ion migration activation energy owing to the strong hydrogen bond interactions. Consequently, (APD)PbI4 SC detectors exhibit high sensitivity (8375 μC Gy−1 cm−2), excellent operating stability, and high-quality X-ray imaging at 1.33 μGy s−1.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6505–6515"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148933301","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

In Situ Polymerizable Lead-Chelating Crown Ether for Lead Leakage Inhibition in Perovskite Solar Cells 钙钛矿太阳能电池中抑制铅泄漏的原位可聚合铅螯合冠醚

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-06-29 DOI: 10.1021/acsenergylett.6c00703

Shichu Peng, Zhixin Liu, Ting Xue, Lida Wang, Wenbo Peng, Jiasheng Zou, Peide Zhu, Bowen Xue, Jiangfeng Wang, Xingzhu Wang, Lei Yan, Liwen Yang, Baomin Xu

{"title":"In Situ Polymerizable Lead-Chelating Crown Ether for Lead Leakage Inhibition in Perovskite Solar Cells","authors":"Shichu Peng, Zhixin Liu, Ting Xue, Lida Wang, Wenbo Peng, Jiasheng Zou, Peide Zhu, Bowen Xue, Jiangfeng Wang, Xingzhu Wang, Lei Yan, Liwen Yang, Baomin Xu","doi":"10.1021/acsenergylett.6c00703","DOIUrl":"10.1021/acsenergylett.6c00703","url":null,"abstract":"While perovskite solar cells (PSCs) have garnered substantial attention owing to the high power conversion efficiency (PCE), light weight, and potential for cost reduction, their long-term stability and the pollution impact on the environment remain significant issues that need to be addressed urgently. The primary challenges in lead-based perovskites are caused by the segregation and migration of Pb2+ within the perovskite grain boundaries (GBs) and interface during device operation, which accelerate the degradation of perovskite and ultimately result in lead leakage. In this research, the stability of perovskite is improved through the in situ polymerization of DVB18C6, a polymerizable crown ether with selective lead chelating property within the perovskite GBs. The robust GBs formed by DVB18C6 optimize perovskite film defects and suppress device lead leakage. The champion device achieved a PCE of 26.78%, with a Pb2+ sequestration efficiency (SQE) of 95.14%. By integrating lead-chelating functionality with polymerizable groups, this approach improves the stability of PSCs and effectively mitigates lead leakage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6456–6465"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148385087","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

Low-Potential Interfacial Oxidation of Piperidinium Ionomers to Formate Contributes to Hydrogen Evolution in AEM Water Electrolyzers Piperidinium离聚体低电位界面氧化生成甲酸盐有助于AEM水电解槽中析氢

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-26 DOI: 10.1021/acsenergylett.6c02584

Sun Young Kang, Heemin Park, Hubert Jedrzej Szabat, Md Estak Ahmed, Piotr Polczynski, Yu Seung Kim

{"title":"Low-Potential Interfacial Oxidation of Piperidinium Ionomers to Formate Contributes to Hydrogen Evolution in AEM Water Electrolyzers","authors":"Sun Young Kang, Heemin Park, Hubert Jedrzej Szabat, Md Estak Ahmed, Piotr Polczynski, Yu Seung Kim","doi":"10.1021/acsenergylett.6c02584","DOIUrl":"10.1021/acsenergylett.6c02584","url":null,"abstract":"Piperidinium-functionalized ionomers are widely used alkaline-stable binders in anion exchange membrane water electrolyzers (AEMWEs). Although oxidative degradation has been demonstrated under strongly polarized, reactive oxygen species (ROS)-generating conditions, whether it can initiate through a distinct low-potential interfacial pathway before appreciable oxygen evolution remained unresolved. Here, we show that piperidinium groups undergo potential-induced interfacial oxidation on IrO2 near 1.3 V vs the reversible hydrogen electrode under deoxygenated conditions, demonstrating that dissolved O2 and diffusible O2-derived oxidants are not required. Quantitative 13C nuclear magnetic resonance spectroscopy identifies formate as the dominant soluble product, accompanied by ion-exchange-capacity loss and damage to a backbone-integrated structural unit. Faradaic-efficiency measurements in a pure-water-fed AEMWE show a 16.9% H2-normalized O2 deficit at 1.6 V, consistent with a substantial non-oxygen evolution reaction (OER) contribution from piperidinium oxidation. These findings distinguish low-potential interfacial oxidation from diffusible-ROS-mediated degradation and establish anodic cation stability as critical to durable pure-water-fed AEMWEs and reliable OER catalyst evaluation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6990–6997"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049807","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