Hongqiang Dong, Jiahao Zhao, Ya Lu, Zhennan Tian, Shumeng Wang, Xuguan Bai, Guanfei Gong, Jike Wang, Lu Wang, Shigui Chen
{"title":"Construction of supramolecular metal-halogen bonded organic frameworks for efficient solar energy conversion","authors":"Hongqiang Dong, Jiahao Zhao, Ya Lu, Zhennan Tian, Shumeng Wang, Xuguan Bai, Guanfei Gong, Jike Wang, Lu Wang, Shigui Chen","doi":"10.1016/j.jechem.2025.04.056","DOIUrl":"10.1016/j.jechem.2025.04.056","url":null,"abstract":"<div><div>Efficient conversion and synergistic solar energy utilization are critical for advancing low-carbon and sustainable development. In this study, two Pt(II)-based metal/halogen-bonded organic frameworks (MXOF-Ben and MXOF-Anth) were designed to enhance photoconversion efficiency and enable multifunctional integration. The ligand L-terpyr is formed by coupling tripyridine with diphenylamine dipyridine, in which the tripyridine effectively acts as a metal-ligand to lower the band gap and promote non-radiative leaps, thereby enhancing the photoconversion ability. Meanwhile, diphenylamine dipyridine serves as a [N⋯I<sup>+</sup>⋯N] halogen-bonding acceptor, imparting superhydrophilicity to the materials and increasing carrier density, further improving photocatalytic performance. Experimental results demonstrate that these two MXOFs achieve impressive interfacial water evaporation efficiencies of up to 87.8% and 94.0%, respectively. Additionally, the materials exhibit excellent performance in photothermal power generation and photocatalysis of H<sub>2</sub>O<sub>2</sub>. Notably, the MXOFs also deliver strong overall performance in integrated systems combining interfacial water evaporation with photothermal power generation or photocatalysis, underscoring their exceptional photoconversion efficiency and multifunctional potential. This work introduces a novel strategy by incorporating metal-ligand and halogen bonds, offering a pathway to enhance photoconversion efficiency and develop versatile materials for advanced solar energy applications, thereby fostering the progress of high-efficiency solar energy conversion and multifunctional organic materials.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 527-535"},"PeriodicalIF":13.1,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072594","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhongyu Liu , Xiu Huang , Yuchen Zhao , Jianwei Wang , Jiaying Liu , Chenyu Zhou , Hongwei Wang , Tian Cui , Xiaohui Liu
{"title":"Self-crosslinking strategy enabling high-performance inverted inorganic perovskite solar cells with fill factor exceeding 85%","authors":"Zhongyu Liu , Xiu Huang , Yuchen Zhao , Jianwei Wang , Jiaying Liu , Chenyu Zhou , Hongwei Wang , Tian Cui , Xiaohui Liu","doi":"10.1016/j.jechem.2025.04.060","DOIUrl":"10.1016/j.jechem.2025.04.060","url":null,"abstract":"<div><div>Inorganic CsPbI<sub>3</sub> perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications. Nevertheless, the power conversion efficiency (PCE) of CsPbI<sub>3</sub> perovskite solar cells (PSCs) still lags far behind that of both organic-inorganic hybrid counterparts and the theoretical PCE limit, primarily restricted by severe fill factor (FF) and open-circuit voltage (<em>V</em><sub>OC</sub>) deficits. Herein, an in-situ self-crosslinking strategy is proposed to construct high-performance inverted inorganic PSCs by incorporating acrylate monomers as additives into CsPbI<sub>3</sub> perovskite precursors. During the thermal annealing process of perovskite films, acrylate monomers can form network structures by breaking the C=C groups through an in-situ polymerization reaction, mainly anchored at the grain boundaries (GBs) and on the surfaces of perovskite. Meanwhile, the C=O groups of acrylate polymers can favorably coordinate with uncoordinated Pb<sup>2+</sup>, thereby decreasing defect density and stabilizing the perovskite phase. Particularly, with multiple crosslinking and passivation sites, the incorporation of dipentaerythritol pentaacrylate (DPHA) can effectively improve the perovskite film quality, suppress nonradiative recombination, and block moisture erosion. Consequently, the DPHA-based PSC achieves a champion PCE of 20.05% with a record-high FF of 85.05%, both of which rank among the top in the performance of inverted CsPbI<sub>3</sub> PSCs. Moreover, the unencapsulated DPHA-based device exhibits negligible hysteresis, remarkably improved long-term storage, and operational stability. This work offers a facile and useful strategy to simultaneously promote the efficiency and device stability of inverted inorganic PSCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 381-389"},"PeriodicalIF":13.1,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rui Xue , Shu Yuan , Rongyi Wang , Tianzi Bi , Guiru Zhang , Huiyuan Li , Jiewei Yin , Liuxuan Luo , Shuiyun Shen , Xiaohui Yan , Junliang Zhang
{"title":"The insights into ionomer-catalyst interactions enabling high-efficiency CO2 electroreduction in pure water","authors":"Rui Xue , Shu Yuan , Rongyi Wang , Tianzi Bi , Guiru Zhang , Huiyuan Li , Jiewei Yin , Liuxuan Luo , Shuiyun Shen , Xiaohui Yan , Junliang Zhang","doi":"10.1016/j.jechem.2025.04.057","DOIUrl":"10.1016/j.jechem.2025.04.057","url":null,"abstract":"<div><div>With the development of renewable energy, electrochemical carbon dioxide reduction reaction (CO<sub>2</sub>RR) has become a potential solution for achieving carbon neutrality. However, until now, due to issues with salt precipitate and regeneration of the electrolyte, this technology faces challenges such as difficulty in maintaining long-term stable operation and excessive costs. The pure water CO<sub>2</sub> electrolyzers are believed to be the ultimate solution to eliminate the salt depreciation and electrolyte issues. This study develops an in-situ method tailored for CO<sub>2</sub> reduction in pure water. By employing distribution of relaxation times (DRT) analysis and in-situ electrochemical active surface area (ECSA) measurements, we carried out a comprehensive investigation into the mass transport and electrochemical active surface area of gas diffusion electrodes (GDE) under pure water conditions. The maximum 89% CO selectivity and high selectivity (>80%) in the range of 0–300 mA/cm<sup>2</sup> were achieved using commercial Ag nanoparticles by rational design of catalyst layer. We found that ionomers influence the CO<sub>2</sub> electrolyzers performance via affecting local pH, GDE-membrane interface, and CO<sub>2</sub> transport, while catalyst loading mainly influences the active area and CO<sub>2</sub> transport. This work provides benchmark and insights for future pure water CO<sub>2</sub> electrolyzers development.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 390-399"},"PeriodicalIF":13.1,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li Liao , Yu Shen , Qinghua Yang , Shuiyong Wang , Mengmeng Yin , Chengcheng Tao , Pan Luo , Jialin Song , Yin Shen , Xuanzhong Wen , Xiaoshuang Luo , Mingshan Wang , Zhenzhong Yang , Xing Li
{"title":"Tailoring and unveiling the stable solvent structure dependence of interfacial chemistry for extremely high-temperature lithium metal batteries","authors":"Li Liao , Yu Shen , Qinghua Yang , Shuiyong Wang , Mengmeng Yin , Chengcheng Tao , Pan Luo , Jialin Song , Yin Shen , Xuanzhong Wen , Xiaoshuang Luo , Mingshan Wang , Zhenzhong Yang , Xing Li","doi":"10.1016/j.jechem.2025.04.055","DOIUrl":"10.1016/j.jechem.2025.04.055","url":null,"abstract":"<div><div>Traditionally, the construction of stable interphases relies on solvent structures dominated by aggregated anionic structures (AGG/AGG+). Nonetheless, we find that the construction of stable interphases in high-temperature environments is based on contact ion pairs (CIPs) dominated solvation structure here. In detail, in the long-chain phosphate ester-based electrolyte, the spatial site-blocking effect enables the strong solvation co-solvent ether (diethylene glycol dimethyl ether, G2) to exhibit strong ion-dipole interactions, further multicomponent competitive coordination maintaining the CIP, balancing electrode kinetics, and optimizing the high-temperature interphases. High-temperature in-situ Raman spectroscopy monitors the changes in the stable solvent structure during charge/discharge processes for the first time, and time of flight secondary ion mass spectrometry (TOF-SIMS) reveals the stable solid electrolyte interphase (SEI) with full-depth enrichment of the inorganic component. Benefiting from the high-temperature interfacial chemistry-dependent solvent structure, the advanced electrolyte enables stable cycling of 1.6 Ah 18650 batterie at 100–125 °C and discharging with high current pulses (∼1.83 A) at 150 °C, which has rarely been reported so far. In addition, pin-pricking of 18650 batteries at 100% state of charge (SoC) without fire or smoke and the moderate thermal runaway temperature (187 °C) tested via the accelerating rate calorimetry (ARC) demonstrate the excellent safety of the optimized electrolyte.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 655-664"},"PeriodicalIF":13.1,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Enhanced buried interface behaviors for high-performance Sn-Pb perovskite solar cells","authors":"Peng Jiang , Qinfei Gao , Jingwei Zhu , Jiayu You , Junyu Qu , Wenbo Jiao , Shenghan Wu , Yuliang Xu , Yuan Xu , Wenwu Wang , Shengqiang Ren , Herui Xi , Canglang Yao , Chuanxiao Xiao , Cong Chen , Dewei Zhao","doi":"10.1016/j.jechem.2025.04.052","DOIUrl":"10.1016/j.jechem.2025.04.052","url":null,"abstract":"<div><div>Numerous defects at the buried interface of perovskite film and the exacerbated oxidation and degradation of tin-lead (Sn-Pb) perovskites induced by poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), due to its hygroscopic and acidic nature, limit performance improvement of Sn-Pb perovskite solar cells (PSCs). To address these issues, 1-Ethyl-3-Guanidinothiourea-Hydrochloride (EGH) was employed as a multifunctional modifier at the PEDOT:PSS/perovskite interface to regulate the buried interface behaviors of Sn-Pb PSCs. EGH can not only passivate the defects of the perovskite buried interface and regulate the work function of PEDOT:PSS for a more matched interface energy level, but also prevent the perovskite film from erosion damage by the acidic PEDOT:PSS for a more stable PEDOT:PSS/perovskite interface. Moreover, the interfacial charge transport dynamics were significantly improved by obviously suppressing interfacial non-radiative recombination losses. As a consequence, EGH-tailored 1.25 eV Sn-Pb PSCs yielded a champion PCE of 23.20%, featuring enhanced long-term stability.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 605-613"},"PeriodicalIF":13.1,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Huijuan Ran , Bingjie Zhou , Leyi Tang , Kehui Wang , Jia Yao , Bo Xiao , Yunfeng Xu , Qing Guo , Erjun Zhou
{"title":"19.1% Efficiency PM6:Y6 based ternary organic solar cells enabled by isomerization engineering of A2-A1-D-A1-A2 type guest molecules","authors":"Huijuan Ran , Bingjie Zhou , Leyi Tang , Kehui Wang , Jia Yao , Bo Xiao , Yunfeng Xu , Qing Guo , Erjun Zhou","doi":"10.1016/j.jechem.2025.04.054","DOIUrl":"10.1016/j.jechem.2025.04.054","url":null,"abstract":"<div><div>In recent years, the ternary strategy of adding a guest molecule to the active layer has been proven to be effective for improving the performance of organic solar cells (OSCs). Isomerization engineering of the guest molecule is a simple method to increase the amount of promising material, but there are only limited reports, and the structure–property relationships are still unclear. In this work, we synthesized three isomers named BTA5-F-<em>o</em>, BTA5-F-<em>m</em>, and BTA5-F-<em>p</em>, with different fluorine substitution positions, to study the influence of isomerization on the photovoltaic performance. After introducing them as the third components to the classic host system PM6:Y6, all three ternary devices showed improved power conversion efficiency (PCEs) compared to the binary system (PCE of 17.46%). The ternary OSCs based on BTA5-F-<em>o</em> achieved a champion PCE of 19.11%, while BTA5-F-<em>m</em> and BTA5-F-<em>p</em> realized PCEs of 18.65% and 18.45%, respectively. Mechanism studies have shown that the dipole moment of the BTA5-F-<em>o</em> end group is closer to that of the Y6 end group, despite the three isomers with almost identical energy levels and optical properties. It is indicated that the electron attraction ability of BTA5-F-o best matches that of Y6, which leads to the higher charge mobility, less charge recombination, and stronger exciton dissociation and extraction ability in the ternary blend system. This study suggests that rationally adjusting the position of substituents in the terminal group can be an effective way to construct nonfullerene guest acceptors to achieve highly efficient ternary OSCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 577-583"},"PeriodicalIF":13.1,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Stepwise energy level regulation via bilayer self-assembled hole-transport materials for efficient and stable inverted perovskite solar cells","authors":"Peng Xu , Xueyan Hou , Xiangnan Sun , Jinping Zhang , Wei Zhang , Xiaoming Zhao","doi":"10.1016/j.jechem.2025.04.051","DOIUrl":"10.1016/j.jechem.2025.04.051","url":null,"abstract":"<div><div>The optimization of hole transport layer (HTL) is crucial for achieving high efficiency and stability in inverted perovskite solar cells (PSCs) due to its role in facilitating hole transport and passivating the perovskite bottom interface. While self-assembled monolayers (SAMs) are commonly used for this purpose, the inherent limitations of a single SAM, such as fixed energy levels and rigid structure, restrict their adaptability for different perovskite components and further efficiency enhancement. Here, we demonstrate a stepwise deposition method for SAM-based HTLs to address this issue. We regulated the energy level gradient by depositing two SAMs with distinct energy levels, while the interactions between the phosphate groups in the SAMs and perovskite effectively reduce defect density at the bottom interface of the perovskite film. The as-fabricated PSCs achieved enhanced efficiency and stability with PCEs of 25.7% and 24.0% for rigid and flexible PSCs, respectively; these devices maintain 90% of their initial PCE after 500 h of maximum power point tracking, and retain 98% of their initial PCE after 4,000 bending cycles, representing one of the most stable flexible PSCs reported to date.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 8-14"},"PeriodicalIF":13.1,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Renming Zhan , Shiyu Liu , Hongyu Luo , Zhengxu Chen , Yangtao Ou, Wenyu Wang, Tianqi Chai, Xiancheng Wang, Shuibin Tu, Zihe Chen, Xiaoxue Chen, Yongming Sun
{"title":"Fast phase transformation of micrometer-scale single-crystal TiNb2O7 anode for Ah-level fast-charging laminated pouch cell","authors":"Renming Zhan , Shiyu Liu , Hongyu Luo , Zhengxu Chen , Yangtao Ou, Wenyu Wang, Tianqi Chai, Xiancheng Wang, Shuibin Tu, Zihe Chen, Xiaoxue Chen, Yongming Sun","doi":"10.1016/j.jechem.2025.04.053","DOIUrl":"10.1016/j.jechem.2025.04.053","url":null,"abstract":"<div><div>The Wadsley-Roth phase TiNb<sub>2</sub>O<sub>7</sub> (TNO) has been identified as a promising anode material with potential for high safety and fast-charging lithium-ion batteries (LIBs), arising from its competitive theoretical specific capacity and secure operational potential. Despite the significant advancements in specific capacity, fast charging, and longevity at the coin cell level, a comprehensive understanding and realization of the fast-charging capability and corresponding cycling stability of the TNO under practical application conditions (such as a pouch cell with an anode capacity exceeding 2 mAh cm<sup>−2</sup>) continues to be elusive. In this study, we explore a simple, scalable solid-phase carbon source melt strategy to fabricate the kilogram-level micrometer-scale single-crystal TNO particles enveloped by an ultrathin carbon coating layer of <5 nm (TNO@C). The in-situ X-ray diffraction (XRD) measurement of the LiCoO<sub>2</sub>||TNO@C laminated pouch cell (anode mass loading of ∼10 mg cm<sup>−2</sup>) under fast charging/discharging conditions with the combination of material characterizations and electrochemical analysis reveals a fast, yet stable crystal structure evolution for the micrometer-scale single-crystal TNO@C with only 7.03% fluctuation in unit cell volume value, which is indicative of fast reaction kinetics. The Ah-level laminated LiCoO<sub>2</sub>||TNO@C pouch cell achieved 80.8% charge within 6 min (10 C) and retained 85.3% capacity after 1000 cycles at the charging current density of 6 C (10 min), far surpassing all the results in previous publications. The straightforward synthetic approach for the micrometer-scale single-crystal TNO@C, coupled with a clear understanding of reaction kinetics and rapid crystal structure evolution, paves the way for the practical application of the micrometer-scale single-crystal TNO@C anode material for fast charging LIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 685-693"},"PeriodicalIF":13.1,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144106103","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Diexin Xie , Jiabin Chen , Jingxin Hou , Fangfang Yang , Runping Feng , Changsheng Cao , Zailai Xie
{"title":"Rational design of oxygen vacancy-rich self-supporting NiCo(OH)2 electrode for efficient biomass upgrading","authors":"Diexin Xie , Jiabin Chen , Jingxin Hou , Fangfang Yang , Runping Feng , Changsheng Cao , Zailai Xie","doi":"10.1016/j.jechem.2025.04.050","DOIUrl":"10.1016/j.jechem.2025.04.050","url":null,"abstract":"<div><div>Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) into high-value 2,5-furandicarboxylic acid (FDCA). However, the rational design of efficient electrocatalysts with precisely tailored structure–activity correlations remains a critical challenge. Herein, we report a hierarchically structured self-supporting electrode (Vo-NiCo(OH)<sub>2</sub>-NF) synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue (NiCo-PBA) precursor, in which oxygen vacancy (Vo)-rich Co-doped Ni(OH)<sub>2</sub> nanosheet arrays are vertically aligned on nickel foam (NF), creating an interconnected conductive network. When evaluated for the HMF oxidation reaction (HMFOR), Vo-NiCo(OH)<sub>2</sub>-NF exhibits exceptional electrochemical performance, achieving near-complete HMF conversion (99%), ultrahigh FDCA Faradaic efficiency (97.5%), and remarkable product yield (96.2%) at 1.45 V, outperforming conventional Co-doped Ni(OH)<sub>2</sub> (NiCo(OH)<sub>2</sub>-NF) and pristine Ni(OH)<sub>2</sub> (Ni(OH)<sub>2</sub>-NF) electrodes. By combining in situ spectroscopic characterization and theoretical calculations, we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers, favor the formation of high-valent Ni<sup>3+</sup> species, and optimize HMF adsorption, thereby improving the HMFOR performance. This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 558-566"},"PeriodicalIF":13.1,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144099250","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xueran Shen , Wenchao Liu , Mingzhe Liu , Haibo Jin , Yuefeng Su , Ning Li , Jingbo Li , Zhiyong Xiong , Caihong Feng , Jianxin Kang , Lin Guo
{"title":"Hard Lewis acid CeO2 and Cl− intercalation induce OH− enriched and strong Cl− repulsive microenvironment for ultra-stable industrialized seawater electrolysis","authors":"Xueran Shen , Wenchao Liu , Mingzhe Liu , Haibo Jin , Yuefeng Su , Ning Li , Jingbo Li , Zhiyong Xiong , Caihong Feng , Jianxin Kang , Lin Guo","doi":"10.1016/j.jechem.2025.04.049","DOIUrl":"10.1016/j.jechem.2025.04.049","url":null,"abstract":"<div><div>Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production, circumventing the constraint of freshwater scarcity. However, the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction (OER) in seawater extremely challenging. Herein, the low-cost and scalable CoFe layered double hydroxides with Cl<sup>−</sup> intercalation and decorated with Ce(OH)<sub>3</sub> (named as CoFe-Cl<sup>−</sup>/Ce(OH)<sub>3</sub>) catalyst is synthesized via rapid electrodeposition under ambient conditions, which is quickly reconstructed into a CeO<sub>2</sub> decorated and Cl<sup>−</sup> intercalated CoFeOOH (CoFeOOH-Cl<sup>−</sup>/CeO<sub>2</sub>) during OER. Theoretical investigation reveals that Cl<sup>−</sup> intercalation weakens the adsorption ability of Cl<sup>−</sup> on Co/Fe atoms and hinders unfavorable coupling with chloride, thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity. The CeO<sub>2</sub> with hard Lewis acidity preferentially binds to OH<sup>−</sup> with harder Lewis base to ensure the OH<sup>−</sup> rich microenvironment around catalyst even under high current operating conditions, thus further enhancing stability and improving OER activity. The functionalized CoFe-Cl<sup>−</sup>/Ce(OH)<sub>3</sub> delivers 1000 mA cm<sup>−2</sup> current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater. Electrochemical experiments elucidate the OER catalytic mechanism in which CeO<sub>2</sub> serves as a co-catalyst for enriching OH<sup>−</sup> and CoFeOOH-Cl<sup>−</sup> is the active species. Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 567-576"},"PeriodicalIF":13.1,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144099251","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}