Journal of Energy Chemistry最新文献

{"title":"Electron-deficient borate anions tailoring the electronic structure of defect-rich amorphous nickel–cobalt cathode for superior capacitive energy storage","authors":"Shaoxiong Du,&nbsp;Wang Yang,&nbsp;Ziyang Cao,&nbsp;Lingyu Kong,&nbsp;Yao Yao,&nbsp;Xi Wu,&nbsp;Tianyu Bai,&nbsp;Chen Zhang,&nbsp;Zhengxuan Li,&nbsp;Yongfeng Li","doi":"10.1016/j.jechem.2025.06.029","DOIUrl":"10.1016/j.jechem.2025.06.029","url":null,"abstract":"<div><div>Designing transition metal nickel–cobalt-based battery-type electrode materials driven by anions is crucial for achieving rapid OH⁻ ion transport under electrochemical activation conditions, thereby improving capacitance performance. Herein, borate anions are selected through theoretical calculations, and two-dimensional (2D) defect-rich amorphous nickel–cobalt-based borate is synthesized via a facile chemical reduction method. Under potentiostatic modification, activated products (NCB-G-E) are obtained. In situ Raman spectra reveal that electron-deficient borate extracts electrons from metal centers, facilitating the oxidation state transition of Ni and Co. Theoretical calculations show that in situ adsorbed borate regulates the d-band centers of metal sites, enhancing OH⁻ intermediate adsorption. Meanwhile, borate anion adsorption accelerates the deprotonation and activation processes. Electrochemical tests demonstrate that NCB-G-E displays superior capacitance performance, with a high quality specific capacity of 383.3 mA h g⁻¹ and 65% retention rate at 30 A g⁻¹, surpassing most nickel–cobalt-based electrodes. The assembled asymmetric supercapacitor presents an impressive energy density of 68.2 Wh kg⁻¹ and good cycling stability. This work highlights the role of electron-deficient borate in tuning metal band structure and promoting oxidation state transition through synergistic defect advantages, offering new prospects for advanced battery-type energy storage materials.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 786-797"},"PeriodicalIF":13.1,"publicationDate":"2025-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535053","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":"Cutting-edge gas sensor design for monitoring thermal runaway in lithium-ion batteries: a critical review","authors":"Jiaojiao Deng ,&nbsp;Xiaoliang Yu ,&nbsp;Dongqing Pang ,&nbsp;Ban Fei ,&nbsp;Jinhan Mo","doi":"10.1016/j.jechem.2025.06.025","DOIUrl":"10.1016/j.jechem.2025.06.025","url":null,"abstract":"<div><div>Thermal runaway (TR) in lithium-ion batteries (LIBs) poses significant safety risks due to its potential to trigger fires and explosions. Early warning of battery TR through gas sensing has emerged as a promising strategy for hazard mitigation. However, comprehensive reviews critically summarizing recent progress in advanced gas sensing technologies remain scarce. To fill this void, we present a critical review consolidating state-of-the-art advancements in gas sensing for TR early warning. This review first overviews the fundamentals of gas sensing for TR monitoring, encompassing thermodynamics and kinetic principles of gas evolution alongside current gas sensing technologies. We then comprehensively explored multi-scale engineering methods, spanning material innovations, device configurations, and system-level integration, with an emphasis on cutting-edge techniques like additive manufacturing and data-driven design frameworks. Future research priorities are identified, including the enhancement of gas selectivity and environmental robustness, the development of machine learning-driven intelligent gas sensing networks, and the establishment of standardized protocols for practical deployment. By integrating interdisciplinary insights derived from materials science, electrochemistry, and embedded systems engineering, this review is positioned to offer actionable guidelines for advancing scalable and reliable gas-sensing solutions toward boosted LIB safety.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 769-785"},"PeriodicalIF":13.1,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514070","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":"Visualizing interfacial charge transfer of two-dimensional heterostructure photocatalyst for efficient CO2 photoreduction via in situ spectroscopies","authors":"Jiusi Shang ,&nbsp;Heng Cao ,&nbsp;Peiyu Ma ,&nbsp;Ruyang Wang ,&nbsp;Jiawei Xue ,&nbsp;Chengyuan Liu ,&nbsp;Guoping Sheng ,&nbsp;Xiaodi Zhu ,&nbsp;Jun Bao","doi":"10.1016/j.jechem.2025.06.023","DOIUrl":"10.1016/j.jechem.2025.06.023","url":null,"abstract":"<div><div>Photocatalytic CO₂ reduction into value-added chemicals holds significant promise for carbon–neutral recycling and solar-to-fuel conversion. Enhancing reaction efficiency by manipulating charge transfer is a key approach to unlocking this potential. In this work, we construct a two-dimensional/two-dimensional (2D/2D) FeSe₂/protonated carbon nitride (FeSe₂/PCN) heterostructure to promote the interfacial charge transfer dynamics, leading to a four-fold improved conversion efficiency of photocatalytic CO₂ reduction with near 100% CO selectivity. Combining in situ X-ray photoelectron spectroscopy, in situ soft X-ray absorption spectroscopy, and femtosecond transient absorption spectroscopy, it is revealed that FeSe₂ acts as an electron acceptor upon photoexcitation, introducing an additional electron transfer pathway from PCN to FeSe₂ that suppresses radiative recombination and promotes charge transfer. In situ X-ray absorption fine structure spectroscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy, and density functional theory calculation further unravel that the electron-enriched FeSe₂ functions as the active sites for CO₂ activation and significantly reduces the energy barrier of key intermediate COOH* formation, which is the rate-determined step for CO generation. This work underscores the importance of regulating photocarrier relaxation pathways to achieve effective spatial charge separation for promoted photocatalytic CO₂ reduction and demonstrates the powerful functions of in situ spectroscopies in in-depth understanding of the photocatalytic mechanism.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 798-806"},"PeriodicalIF":13.1,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535054","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":"Engineering core–shell-structured BaAl2O4 overlaid Ni catalyst with strong metal-support interaction for durable and efficient CH4 dry reforming","authors":"Qiangqiang Xue ,&nbsp;Kang Hui Lim ,&nbsp;Zhehao Sun ,&nbsp;Binhang Yan ,&nbsp;Zongyou Yin ,&nbsp;Ange Nzihou ,&nbsp;Yujun Wang ,&nbsp;Guangsheng Luo ,&nbsp;Feng-Shou Xiao ,&nbsp;Sibudjing Kawi","doi":"10.1016/j.jechem.2025.06.024","DOIUrl":"10.1016/j.jechem.2025.06.024","url":null,"abstract":"<div><div>Dry reforming of methane (DRM) over Ni-based catalysts is an economically reasonable technology for large-scale CO₂ utilization. However, prolonged Ni sintering and carbon deposition reduce the durability and efficiency of DRM, hindering its engineering application. Herein, we propose a facile approach by combining continuous microscale coprecipitation with solid-state reactions to construct a BaAl₂O₄-overlayer-confined Ni catalyst. The 5- wt%-Ni@BaAl₂O₄ catalyst exhibited advanced CO₂ and CH₄ conversions of 96% and 86% at 800 °C and a GHSV of 144 L g_cat.⁻¹ h⁻¹. Moreover, the <em>k</em>_d-CO₂ and <em>k</em>_d-CH₄ of Ni@BaAl₂O₄ were 0.0063 and 0.0029 h⁻¹; which are approximately half and one-thirds of those of Ni/BaAl₂O₄ and slightly better than those of Ni@MgAl₂O₄, underscoring the versatility of the proposed synthesis protocol for constructing core–shell structures. XAS, HAADF–STEM–EDS, and CO transmission-IR characterizations confirmed the SMSI of ∼2-nm amorphous BaAl₂O₄-overlaid ∼10 nm Ni with an overall mesoporous structure. After a long-term test, the sintering and coking inhibition effects of Ni@BaAl₂O₄ (10 → 11 nm, 0.55 mg_C g_cat.⁻¹ h⁻¹) outperformed Ni/BaAl₂O₄ (13 → 22 nm, 1.90 mg_C g_cat.⁻¹ h⁻¹) and Ni@MgAl₂O₄. In situ time-resolved CH₄ → CO₂ transient response, DRIFTS experiments, and DFT calculations suggested that Ni@BaAl₂O₄ and Ni/BaAl₂O₄ followed the Mars–van Krevelen and Langmuir–Hinshelwood redox mechanisms, respectively. The functional interfacial lattice oxygen promoted the removal of C_ads* on Ni and core–shell structure induced fast CO₂ adsorption and CO desorption. The present study provides a facile approach for constructing a stable and active Ni-based core − shell catalyst. Furthermore, it offers novel insights into the functionalities of non-reducible spinel overlayers in the DRM process.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 807-819"},"PeriodicalIF":13.1,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535055","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":"Spin and orbital manipulation of multiple atomic sites by high-entropy effect for catalyzing cascade sulfur conversion","authors":"Weihao Gong ,&nbsp;Guangfu Dai ,&nbsp;Hongjiao Liu ,&nbsp;Haobo Sun ,&nbsp;Zeyi Wu ,&nbsp;Xinpeng Zhao ,&nbsp;Haoting Miao ,&nbsp;Ying Jiang ,&nbsp;Zhengqing Ye","doi":"10.1016/j.jechem.2025.06.017","DOIUrl":"10.1016/j.jechem.2025.06.017","url":null,"abstract":"<div><div>Lithium-sulfur (Li-S) batteries are considered a potential candidate for next-generation energy-dense and sustainable energy storage. However, the slow conversion and severe shuttle of polysulfides (LiPSs) result in rapid performance degradation over long-term cycling. Herein, we report a high-entropy single-atom (HE-SA) catalyst to regulate the multi-step conversion of LiPS to attain a high-performance Li-S battery. Both the density functional theory calculations and the experimental results prove that the Fe atomic site with high spin configurations strongly interacts with Li₂S₄ through <em>d</em>-<em>p</em> and <em>s</em>-<em>p</em> synergistic orbital hybridization which facilitates the reduction of LiPS. Moreover, S-dominant <em>p</em>-<em>d</em> hybridization between Li₂S and a high-spin Mn site weakens the Li–S bond and facilitates the rapid sulfur evolution reaction. Consequently, the Li-S battery with a bifunctional HE-SA catalyst shows an ultralow capacity decay of 0.026 % per cycle over 1900 cycles at 1 C. This work proposes a high-entropy strategy for sculpting electronic structures to enable spin and orbital hybridization modulation in advanced catalysts toward long-cycling Li-S batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 671-680"},"PeriodicalIF":13.1,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144491527","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":"Printable hole-conductor-free mesoscopic perovskite solar cells coupled with an ultra-thin ZrO2 interface layer for improved performance","authors":"Kai Chen ,&nbsp;Jinwei Gong ,&nbsp;Jiale Liu,&nbsp;Jianhang Qi,&nbsp;Qiaojiao Gao,&nbsp;Yongming Ma,&nbsp;Yanjie Cheng,&nbsp;Wenjing Hu,&nbsp;Junwei Xiang,&nbsp;Anyi Mei,&nbsp;Hongwei Han","doi":"10.1016/j.jechem.2025.06.018","DOIUrl":"10.1016/j.jechem.2025.06.018","url":null,"abstract":"<div><div>Modulating the interface between the electron transport layer (ETL) and perovskite to minimize interfacial recombination is pivotal for developing efficient and stable perovskite solar cells. Here, we introduce an ultra-thin ZrO₂ insulating interface layer onto the inner surface of the mesoporous TiO₂ ETL via the chemical bath deposition in the zirconium n-butoxide solution, which alters the interface characteristics between TiO₂ and perovskite for the printable hole-conductor-free mesoscopic perovskite solar cells (p-MPSCs). The insulating ZrO₂ interface layer reduces interface defects and suppresses interfacial non-radiative recombination. Furthermore, the ZrO₂ interface layer improves the wettability of the mesoporous TiO₂ ETL, which favors the crystallization of perovskite within the mesoporous scaffold. Meanwhile, the device performance presents thickness dependence on the interface layer. While increased thickness improves the open-circuit voltage, excessive thickness negatively impacts both the short-circuit current density and fill factor. Consequently, an improved power conversion efficiency of 19.9% was achieved for p-MPSCs with the ZrO₂ interface layer at its optimized thickness.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 762-768"},"PeriodicalIF":13.1,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144502480","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 thermal robustness of NCM-LATP composite cathodes via in situ lithium compensators for co-sintering","authors":"Lifan Wang ,&nbsp;Pengfei Jiang ,&nbsp;Ruixiang Li ,&nbsp;Xindong Wang ,&nbsp;Chun Zhan ,&nbsp;Guicheng Liu","doi":"10.1016/j.jechem.2025.06.014","DOIUrl":"10.1016/j.jechem.2025.06.014","url":null,"abstract":"<div><div>Composite cathodes integrating Ni-rich layered oxides and oxide solid electrolytes are essential for high-energy all-solid-state lithium-ion batteries (ASSLBs), yet interfacial degradation during high-temperature co-sintering (&gt;600 °C) remains a critical challenge. While surface passivation strategies mitigate reactions below 400 °C, their effectiveness diminishes at elevated temperatures due to inability to counteract Li⁺ concentration gradients. Here, we introduce in situ lithium compensators, i.e., LiOH/Li₂CO₃, into NCM-LATP composite cathodes to dynamically replenish Li⁺ during co-sintering. These additives melt to form transient Li⁺-rich phases that back-diffuse Li⁺ into NCM lattices, suppressing layered-to-rock salt transitions and stabilizing the interface. Quasi in situ XRD confirms retention of the layered structure at temperature up to 700 °C, while electrochemical tests demonstrate a reversible capacity of 222.2 mA h g⁻¹—comparable to NCM before co-sintering—and an impressive 65.3% capacity retention improvement over 100 cycles. In contrast, uncompensated cathodes exhibit severe degradation to 96.5 mA h g⁻¹ due to Li depletion and resistive Li-Ti-O interphases. This strategy integrates sacrificial chemistry with scalable powder-mixing workflows, achieving a 93.4% reduction in interfacial impedance. By addressing Li⁺ flux homogenization and structural stability, this work provides a practical pathway toward industrial-scale fabrication of high-performance ASSLBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 749-761"},"PeriodicalIF":13.1,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144502455","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":"Enhancing power capability and fast discharge behavior in P2-type K layered cathodes through structural stabilization via introducing Li-ions into TM layers","authors":"Hyunji Kweon ,&nbsp;Jungmin Kang ,&nbsp;Bonyoung Ku ,&nbsp;Sunha Hwang ,&nbsp;Jinho Ahn ,&nbsp;Lahyeon Jang ,&nbsp;Myungeun Choi ,&nbsp;Sang-Yeop Lee ,&nbsp;Jihoe Lee ,&nbsp;Hoseok Lee ,&nbsp;Hun-Gi Jung ,&nbsp;Jang-Yeon Hwang ,&nbsp;Hee-Dae Lim ,&nbsp;Jongsoon Kim","doi":"10.1016/j.jechem.2025.06.019","DOIUrl":"10.1016/j.jechem.2025.06.019","url":null,"abstract":"<div><div>Mn-based layered oxides are widely recognized as cathode materials for potassium-ion batteries (KIBs) due to their high specific capacity derived from their low molar mass. However, the structural instability caused by the Jahn-Teller effect of Mn³⁺ and the large ionic radius of K⁺ results in poor electrochemical performance. Herein, we propose an effective structural stabilization strategy for P2-type Mn-based layered oxide cathodes of KIBs through Li-incorporation into the transition metal layer. Using the first-principles calculations and experiments, we demonstrate that the P2-K_0.48[Li_0.1Mn_0.9]O₂ (P2-KLMO) delivers improved electrochemical performance, specific capacity and average discharge voltage of ∼124.4 mA h g⁻¹ and ∼2.7 V (vs. K⁺/K) at 0.05C (1C = 260 mA g⁻¹), outperforming P2-K_0.5MnO₂. <em>Operando</em> X-ray diffraction analysis confirms the P2-OP4 phase transition and Mn³⁺-induced Jahn-Teller distortion are significantly suppressed in P2-KLMO. These improvements are attributed to the lithium introduction into transition metal layers, leading to strengthened structural stability and enhanced K⁺ diffusion kinetics. Moreover, synthetic accessibility through the conventional solid-state method provides an additional advantage for practical application of Li-incorporated Mn-based P2-type cathodes in KIBs. We believe our study offers a simple yet effective strategy for designing high-performance and practical cathode materials for KIBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 820-829"},"PeriodicalIF":13.1,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144535056","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":"Rational design of MXene@VS4 heterostructures via interfacial coupling for advanced magnesium-ion batteries","authors":"Xinyu Zhang ,&nbsp;Wenxin Li ,&nbsp;Meihan Sun ,&nbsp;Meng Wu ,&nbsp;Fanfan Liu ,&nbsp;Dan Zhou","doi":"10.1016/j.jechem.2025.06.011","DOIUrl":"10.1016/j.jechem.2025.06.011","url":null,"abstract":"<div><div>Rechargeable magnesium batteries (RMBs) have garnered significant attention in energy storage applications due to their high capacity, low cost, and high safety. However, the strong polarization effect and slow kinetic de-intercalation of Mg²⁺ in the cathode limit their commercial application. This study presents a novel interface-coupled V₂CT<em>_x</em>@VS₄ heterostructure through a one-step hydrothermal process. In this architecture, V₂CT<em>_x</em> and VS₄ can mutually support their structural framework, which effectively prevents the structural collapse of V₂CT<em>_x</em> MXene and the aggregation of VS₄. Crucially, interfacial coupling between V₂CT<em>_x</em> and VS₄ induces strong V–S bonds, substantially enhancing structural stability. Benefiting from these advantages, the heterostructure exhibits high specific capacity (226 mAh g⁻¹ at 100 mA g⁻¹) and excellent long-cycle stability (89% capacity retention after 1000 cycles at 500 mA g⁻¹). Furthermore, the Mg²⁺ storage mechanism in the V₂CT<em>_x</em>@VS₄ composite was elucidated through a series of ex-situ characterizations. This work provides a feasible strategy for designing V₂CT<em>_x</em> MXene-based cathodes with high capacity and extended cyclability for RMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 566-575"},"PeriodicalIF":13.1,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144365044","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":"Atomic vacancy engineering of Co(OH)F nanoarray toward high-performance ammonia electrosynthesis with waste plastics upgrading","authors":"Mingdan Wang ,&nbsp;Qianyu Zhang ,&nbsp;Kun Chen ,&nbsp;Cong Lin ,&nbsp;Huigang Wang ,&nbsp;Yanying Zhao ,&nbsp;Pengzuo Chen","doi":"10.1016/j.jechem.2025.06.012","DOIUrl":"10.1016/j.jechem.2025.06.012","url":null,"abstract":"<div><div>Developing energy-efficient nitrite-to-ammonia (NO₂RR) conversion technologies while simultaneously enabling the electrochemical upcycling of waste polyethylene terephthalate (PET) plastics into high-value-added chemicals is of great significance. Herein, an atomic oxygen vacancy (V_o) engineering is developed to optimize the catalytic performance of V_o2-Co(OH)F nanoarray towards the NO₂RR and PET-derived ethylene glycol oxidation reaction (EGOR). The optimal V_o2-Co(OH)F achieves an ultralow operating potential of −0.03 V vs. RHE at −100 mA cm⁻² and a remarkable NH₃ Faradaic efficiency (FE) of 98.4% at −0.2 V vs. RHE for NO₂RR, and a high formate FE of 98.03% for EGOR. Operando spectroscopic analysis and theoretical calculations revealed that oxygen vacancies play a crucial role in optimizing the electronic structure of V_o2-Co(OH)F, modulating the adsorption free energies of key reaction intermediates, and lowering the reaction energy barrier, thereby enhancing its overall catalytic performance. Remarkably, the V_o2-Co(OH)F-based NO₂RR||EGOR electrolyzer realized high NH₃ and formate yield rates of 33.9 and 44.9 mg h⁻¹ cm⁻² at 1.7 V, respectively, while demonstrating outstanding long-term stability over 100 h. This work provides valuable insights into the rational design of advanced electrocatalysts for co-electrolysis systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 558-565"},"PeriodicalIF":13.1,"publicationDate":"2025-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144331039","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}