Journal of Energy Chemistry最新文献

A large-scale on-the-fly machine learning molecular dynamics simulation to explore lithium metal battery interfaces 大规模实时机器学习分子动力学模拟，探索锂金属电池界面

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-09 DOI: 10.1016/j.jechem.2025.06.072

Yi-Lin Niu , Xiang Chen , Tian-Chen Zhang , Yu-Chen Gao , Yao-Peng Chen , Nan Yao , Zhong-Heng Fu , Qiang Zhang

{"title":"A large-scale on-the-fly machine learning molecular dynamics simulation to explore lithium metal battery interfaces","authors":"Yi-Lin Niu , Xiang Chen , Tian-Chen Zhang , Yu-Chen Gao , Yao-Peng Chen , Nan Yao , Zhong-Heng Fu , Qiang Zhang","doi":"10.1016/j.jechem.2025.06.072","DOIUrl":"10.1016/j.jechem.2025.06.072","url":null,"abstract":"<div><div>The global rapid transition towards sustainable energy systems has heightened the demand for high-performance lithium metal batteries (LMBs), where understanding interfacial phenomena is paramount. In this contribution, we present an on-the-fly machine learning molecular dynamics (OTF-MLMD) approach to probe the complex side reactions at lithium metal anode–electrolyte interfaces with exceptional accuracy and computational efficiency. The machine learning force field (MLFF) was firstly validated in a bulk-phase system comprising twenty 1,2-dimethoxyethane (DME) molecules, demonstrating energy fluctuations and structural parameters in close agreement with <em>ab initio</em> molecular dynamics (AIMD) benchmarks. Subsequent simulations of lithium–DME and lithium–electrolyte interfaces revealed minimal discrepancies in energy, bond lengths, and net charge variations (notably in FSI<sup>−</sup> species), underscoring the method’s DFT-level precision of the approach. A further small-scale interfacial model enabled on-the-fly training over a mere of 340 fs, which was then successfully transferred to a large-scale simulation encompassing nearly 300,000 atoms, representing the largest interfacial model in LMB research up to date. The hierarchical validation strategy not only establishes the robustness of the MLFF in capturing both interfacial and bulk-phase chemistry but also paves the way for statistically meaningful simulations of battery interfaces. The fruitful findings highlight the transformative potential of OTF-MLMD in bridging the gap between atomistic accuracy and macroscopic modeling, affording a universal approach to understand interfacial reactions in LMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 356-362"},"PeriodicalIF":13.1,"publicationDate":"2025-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678986","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}

引用次数: 0

Identifying interface evolutions for achieving stable solid-state Li metal batteries 确定实现稳定固态锂金属电池的界面演变

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-07 DOI: 10.1016/j.jechem.2025.06.070

Peng Chen, Peilin Guo, Weijian Guo, Bing Ding, Hui Dou, Xiaogang Zhang

{"title":"Identifying interface evolutions for achieving stable solid-state Li metal batteries","authors":"Peng Chen, Peilin Guo, Weijian Guo, Bing Ding, Hui Dou, Xiaogang Zhang","doi":"10.1016/j.jechem.2025.06.070","DOIUrl":"10.1016/j.jechem.2025.06.070","url":null,"abstract":"<div><div>Solid-solid interface contact and slow ion transport restrict solid-state polymer electrolytes practical application. The differences in interface structure design significantly influence the interfacial Li<sup>+</sup> transport and diffusion as well as the Li atom nucleation, resulting in substantial variations in the macroscopic performance of polymer electrolytes-based solid-state Li metal batteries. Here, ceramic-polymer composite electrolytes (CPCEs) composed of polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) polymer and Li<sub>6.75</sub>La<sub>3</sub>Zr<sub>1.75</sub>Ta<sub>0.25</sub>O<sub>12</sub> (LLZTO) filler has been chosen as the demo to demonstrate that the interfacial electrochemistry between CPCEs and Li anode is not only affected by the physical interface contact but also associated with the internal/interfacial Li<sup>+</sup> transport mechanism. This work shows that “point to point” Li<sup>+</sup> diffusion, slow uneven interfacial Li<sup>+</sup> transport in CPCEs with poor ionic conductivity and rough surface lead to uneven Li atom nucleation, leading to Li dendrites growth. While, the CPCEs with high ionic conductivity and smooth surface facilitate uniform and rapid ion transport, promoting uniform Li nucleation and transverse diffusion. This work highlights the importance of the interface structure design of polymer electrolytes for Li metal interface stability in polymer electrolytes-based quasi-solid-state batteries and provides valuable insights into the interfacial electrochemistry of solid-state batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 363-371"},"PeriodicalIF":13.1,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678954","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}

引用次数: 0

Design strategies for enhancing the synthesis of C3+ products from electrochemical CO2 reduction 提高CO2电化学还原合成C3+产物的设计策略

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-07 DOI: 10.1016/j.jechem.2025.06.067

Yan Huang , De-Sheng Zheng , Wen-Chuan Lai , Zhi-Yuan Gu

{"title":"Design strategies for enhancing the synthesis of C3+ products from electrochemical CO2 reduction","authors":"Yan Huang , De-Sheng Zheng , Wen-Chuan Lai , Zhi-Yuan Gu","doi":"10.1016/j.jechem.2025.06.067","DOIUrl":"10.1016/j.jechem.2025.06.067","url":null,"abstract":"<div><div>The electrochemical CO<sub>2</sub> reduction reaction (eCO<sub>2</sub>RR) offers significant potential for closing the anthropogenic carbon cycle while simultaneously enabling the storage of intermittent sustainable energy. The synthesis of C<sub>3+</sub> products from eCO<sub>2</sub>RR is particularly appealing due to their higher commercial value compared to C<sub>1</sub> or C<sub>2</sub> compounds, and their crucial roles as high-energy-density fuels or feedstocks for a wide range of industrial applications. This encourages us to summarize recent notable progress in enhancing C<sub>3+</sub> production. This review starts from the formation pathways of C<sub>3+</sub> products by delving into key intermediates and *C–*C coupling reactions for mechanistic investigations. Subsequently, we discuss the representative eCO<sub>2</sub>RR electrocatalysts for C<sub>3+</sub> synthesis, including Cu and non-Cu catalysts, highlighting typical design strategies for markedly promoting the catalytic performance or expanding the range of products. Additionally, we also emphasize system upgrading strategies, covering manipulation of electrolysis conditions, microenvironment regulation, and cascade catalysis, for facilitating C<sub>3+</sub> production. We finally end with future directions in this rapidly advancing field. By elucidating the formation mechanisms, catalyst design principles, and system upgrading strategies, this review is expected to draw significant attention to C<sub>3+</sub> products and stimulate further research into developing advanced catalytic systems for their efficient synthesis.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 197-218"},"PeriodicalIF":13.1,"publicationDate":"2025-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663471","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}

引用次数: 0

Hydrophobic interface engineering of nickel hydroxide for efficient electrocatalytic fatty alcohol oxidation coupled with hydrogen production 氢氧化镍高效电催化脂肪醇氧化偶联制氢的疏水界面工程

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-05 DOI: 10.1016/j.jechem.2025.06.063

Ruiqi Du, Rui Jia, Bingjie Yuan, Zemao Chen, Kaizheng Zhang, Kaiqi Nie, Binhang Yan, Yi Cheng

{"title":"Hydrophobic interface engineering of nickel hydroxide for efficient electrocatalytic fatty alcohol oxidation coupled with hydrogen production","authors":"Ruiqi Du, Rui Jia, Bingjie Yuan, Zemao Chen, Kaizheng Zhang, Kaiqi Nie, Binhang Yan, Yi Cheng","doi":"10.1016/j.jechem.2025.06.063","DOIUrl":"10.1016/j.jechem.2025.06.063","url":null,"abstract":"<div><div>Electrocatalysis has emerged as a sustainable approach for the selective oxidation of fatty alcohols to fatty acids, circumventing the environmental concerns associated with conventional routes. However, the low aqueous solubility of hydrophobic fatty alcohols presents a major challenge. While nickel hydroxide (Ni(OH)<sub>2</sub>) serves as a cost-effective catalyst for alcohol oxidation, its hydrophilic nature limits substrate accessibility and mass transport, causing sluggish kinetics and competing oxygen evolution. Herein, we propose a hydrophobic interface engineering strategy via co-electrodeposition of Ni(OH)<sub>2</sub> with polytetrafluoroethylene (PTFE), fabricating the composite electrode (ED-Ni(OH)<sub>2</sub>-PTFE). The optimized electrode achieves 95 % Faradaic efficiency for octanoic acid at 1.5 V vs. RHE, with a production rate 2–3 times higher than pristine Ni(OH)<sub>2</sub>. Mechanistic studies combining in situ Raman spectroscopy, fluorescence imaging, and coarse-grained molecular dynamics simulations reveal that PTFE selectively enriches octanol at the electrode-electrolyte interface by modulating interfacial hydrophobicity. A continuous-flow microreactor integrating anodic octanol oxidation with cathodic hydrogen evolution reduces cell voltage by ∼100 mV, achieving simultaneous fatty acid and hydrogen production. This work highlights the critical role of hydrophobic interfacial microenvironment design in organic electrosynthesis, offering a promising strategy for upgrading fatty alcohols under mild conditions.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 255-262"},"PeriodicalIF":13.1,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663474","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}

引用次数: 0

Probing unsuitability of ruthenium dioxide and constructing medium-entropy alloy oxide for polyethylene terephthalate electrocatalytic upcycling 探讨二氧化钌在聚对苯二甲酸乙二醇酯电催化升级回收中的不适用性及构建中熵氧化合金

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-05 DOI: 10.1016/j.jechem.2025.06.061

Xinjie Xie , Chunyong Zhang , Shuang Dong , Zhiqian Zhang , Zhou Yang

{"title":"Probing unsuitability of ruthenium dioxide and constructing medium-entropy alloy oxide for polyethylene terephthalate electrocatalytic upcycling","authors":"Xinjie Xie , Chunyong Zhang , Shuang Dong , Zhiqian Zhang , Zhou Yang","doi":"10.1016/j.jechem.2025.06.061","DOIUrl":"10.1016/j.jechem.2025.06.061","url":null,"abstract":"<div><div>Environmental pollution and energy crisis are the most important problems all over the world. Polyethylene terephthalate (PET) is a widely used and difficult-to-degrade plastic that can be decomposed into terephthalic acid (PTA) and ethylene glycol (EG), and the EG can be electrocatalytically oxidized to high-value-added formic acid (FA). However, the commercial RuO<sub>2</sub> cannot support the EG oxidative reaction (EGOR) due to its strong absorption of intermediates and less exposed active sites, so the RuSb<sub>0.92</sub>O<sub>1.76</sub> medium-entropy alloy oxide (MEAO) was constructed in this work. The RuSb<sub>0.92</sub>O<sub>1.76</sub> fills up the O vacancy of RuO<sub>2</sub> and repairs the instability of RuO<sub>2</sub>, and the lattice O in the RuSb<sub>0.92</sub>O<sub>1.76</sub> promotes the EGOR by sacrificing itself to generate O vacancies. The RuSb<sub>0.92</sub>O<sub>1.76</sub> shows a low EGOR potential of 1.13 V at 10 mA cm<sup>−2</sup>, and a low hydrogen evolution reaction (HER) potential of 43 mV at 10 mA cm<sup>−2</sup>. The RuSb<sub>0.92</sub>O<sub>1.76</sub> shows a high Faradic efficiency (<em>FE</em>) of close to 100 % through the glycolaldehyde/GA pathway via the in situ ATR-IR spectroscopy. Density functional theory (DFT) reveals that RuSb<sub>0.92</sub>O<sub>1.76</sub> has a moderate adsorption capacity for intermediates in the EGOR. This work provides a potential avenue for the MEAO catalysts in electrocatalytic plastic upcycling coupling hydrogen energy.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 219-226"},"PeriodicalIF":13.1,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663472","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}

引用次数: 0

Dynamic modulation of Pt 5d valence electrons by single-atom Cu for boosted alkaline hydrogen evolution catalysis 单原子Cu对p5d价电子的动态调制促进碱性析氢催化

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-05 DOI: 10.1016/j.jechem.2025.06.066

Pengfei Wu , Yuzhuo Sun , Wenjing Miao , Zhaoqin Chu , Jingtian Hu , Yukun Gao , Penggang Yin , Wenxing Chen , Lingling Guo , Degao Wang

{"title":"Dynamic modulation of Pt 5d valence electrons by single-atom Cu for boosted alkaline hydrogen evolution catalysis","authors":"Pengfei Wu , Yuzhuo Sun , Wenjing Miao , Zhaoqin Chu , Jingtian Hu , Yukun Gao , Penggang Yin , Wenxing Chen , Lingling Guo , Degao Wang","doi":"10.1016/j.jechem.2025.06.066","DOIUrl":"10.1016/j.jechem.2025.06.066","url":null,"abstract":"<div><div>Developing efficient and durable alkaline hydrogen evolution reaction (HER) catalysts is crucial for realizing high-performance, practical anion exchange membrane water electrolyzer (AEMWE) operating at ampere-level current densities. Although atomically dispersed Platinum (Pt) catalysts offer significant potential for enhancing atom utilization, their HER performance and durability are limited by the inflexibility in valence electron transfer between Pt and the support. In this study, we utilize asymmetrically single-atom copper (Cu) with tunable valence states as a valence electron reservoir (VER) to dynamically regulate the Pt 5<em>d</em> valence states, achieving efficient alkaline HER. In situ synchrotron radiation and theoretical calculations demonstrate that the dynamic evolution of the Pt 5<em>d</em> valence electron configuration optimizes the adsorption strengths of reaction intermediates. Meanwhile, single-atom Cu accelerates the rate-limiting water dissociation, and Pt facilitates subsequent *H coupling. The catalyst requires only 23.5 and 177.2 mV overpotentials to achieve current densities of 10 and 500 mA cm<sup>−2</sup> in 1 M KOH. Notably, the PtCu/NC exhibits a ∼57 % lower hydrogen evolution barrier than Pt/NC. Moreover, the PtCu/NC-based AEMWE operates for over 600 h at an industrially relevant current density of 500 mA cm<sup>−2</sup>.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 372-381"},"PeriodicalIF":13.1,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678955","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}

引用次数: 0

Doping or loading: unraveling the optimal anchoring strategy of single metal atom on Co3O4 for electrochemical nitrate reduction reaction 掺杂或负载：揭示电化学硝酸还原反应中单个金属原子在Co3O4上的最佳锚定策略

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-05 DOI: 10.1016/j.jechem.2025.06.060

Riming Hu , Haoyu Wang , Ruochen Zhu , Xinyuan Yang , Xiuxian Zhao , Fahao Ma , Jiayuan Yu , Xuchuan Jiang

{"title":"Doping or loading: unraveling the optimal anchoring strategy of single metal atom on Co3O4 for electrochemical nitrate reduction reaction","authors":"Riming Hu , Haoyu Wang , Ruochen Zhu , Xinyuan Yang , Xiuxian Zhao , Fahao Ma , Jiayuan Yu , Xuchuan Jiang","doi":"10.1016/j.jechem.2025.06.060","DOIUrl":"10.1016/j.jechem.2025.06.060","url":null,"abstract":"<div><div>Developing efficient electrocatalysts for the nitrate reduction reaction (NIRR) to ammonia is vital for environmental remediation and sustainable ammonia synthesis. Metal-oxide-based single-atom catalysts (SACs) offer atomic-scale efficiency, yet unclear anchoring strategies for single metal sites hinder their rational design. This study systematically explored the effects of surface-loading and lattice-doping strategies on anchoring transition, rare-earth, and main-group metal atoms onto Co<sub>3</sub>O<sub>4</sub> via the synergy of machine learning and density functional theory calculations. Through a comprehensive assessment of stability, catalytic activity, and electronic structures, it is discovered that lattice-doping enhances SACs stability by firmly anchoring metal atoms on Co sites, while surface-loading significantly boosts catalytic activity for the NIRR. Calculations predicted that Al, Ir, Rh, and Mo sites anchored through the surface-loading strategy exhibited exceptional NIRR activity (the limiting potential for Al site can reaches −0.25 V versus the reversible hydrogen electrode), far surpassing many other configurations. To further decipher the underlying mechanisms, the machine learning algorithms, especially the tree-based pipeline optimization tool model, revealed that SACs activity is highly correlated with the local environment of the active center, particularly its electronic and structural characteristics. This work establishes a new design paradigm for SACs, providing both theoretical guidelines for anchoring strategy selection and a predictive framework for efficient NIRR electrocatalysts.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 336-346"},"PeriodicalIF":13.1,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678984","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}

引用次数: 0

Fire safety challenge of lithium metal batteries and advanced strategies for improving intrinsic safety 锂金属电池的消防安全挑战及提高本质安全的先进策略

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-05 DOI: 10.1016/j.jechem.2025.06.065

Yuan Cheng , Lihua Jiang , Xiangming Hu , Zhiyuan Yang , Hengyu Xu , Biao Kong , Yurui Deng , Longfei Han , Mengdan Zhang , Xiaoxuan Wei , Qingsong Wang

{"title":"Fire safety challenge of lithium metal batteries and advanced strategies for improving intrinsic safety","authors":"Yuan Cheng , Lihua Jiang , Xiangming Hu , Zhiyuan Yang , Hengyu Xu , Biao Kong , Yurui Deng , Longfei Han , Mengdan Zhang , Xiaoxuan Wei , Qingsong Wang","doi":"10.1016/j.jechem.2025.06.065","DOIUrl":"10.1016/j.jechem.2025.06.065","url":null,"abstract":"<div><div>The high energy density of lithium metal batteries (LMBs) has attracted widespread attention, which is expected to improve the endurance mileage of electric vehicles comparable to fossil fuel-powered vehicles. At present, the main research is focused on developing advanced materials and revealing the in-depth electrochemical mechanism of LMBs, while there is a significant lagging behind of attention to the safety evaluation. This review aims to emphasize the fire safety challenges faced by LMBs and summarize advanced strategies for improving intrinsic safety. Firstly, the basic chemical composition and working principle of LMBs were introduced compared with lithium-ion batteries. Moreover, we reviewed the thermal runaway problem of LMBs from the aspects of material activity, interfacial stability triggering conditions, thermal runaway behavior and mechanism, the special thermal runaway characteristics, and new safety challenges of Li-S, Li-O<sub>2</sub>, and the solid-state LMBs were discussed in detail. Based on the analysis of the thermal runaway mechanism, we summarized the advanced strategies, including electrolyte design, interphase film construction, separator, and anode design for improving the intrinsic safety of LMBs. Finally, we proposed the fire safety challenge at the battery level and emphasized the necessity of designing safe materials based on the thermal runaway mechanism. Blocking the thermal coupling reaction and conducting multi-strategy collaborative optimization is the key point to restrain thermal runaway.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 311-335"},"PeriodicalIF":13.1,"publicationDate":"2025-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144679107","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}

引用次数: 0

Manipulating local environment and spin-state of single-atom via helical structure for CO2 electroreduction to formate 通过螺旋结构控制局部环境和单原子自旋状态，使CO2电还原生成

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-04 DOI: 10.1016/j.jechem.2025.06.059

Liuliu Zhu, Huiyan Ren, Hongbo Gu

{"title":"Manipulating local environment and spin-state of single-atom via helical structure for CO2 electroreduction to formate","authors":"Liuliu Zhu, Huiyan Ren, Hongbo Gu","doi":"10.1016/j.jechem.2025.06.059","DOIUrl":"10.1016/j.jechem.2025.06.059","url":null,"abstract":"<div><div>The underappreciated role of supports has severely constrained the modification of single-atom catalysts. It’s important to develop a strategy for achieving a strong synergy between catalytic structures and active sites. Here, we devise a structure-inducing method involving the manipulation of the chemical reaction environment and spin-state of Cu single-atom with helical carbon nanotube (HCNT) for CO<sub>2</sub> efficient electroreduction to formate. Utilizing in situ characterization and finite element simulation, we find that the helical structure effectively enriches HCO<sub>3</sub><sup>−</sup> and OH<sup>−</sup> on the surface of Cu-N<sub>2</sub>O<sub>2</sub>/HCNT catalyst during electrocatalytic CO<sub>2</sub> reduction, creating a favorable interfacial environment for formate generation. Magnetic characterizations and theoretical calculations reveal spin polarization of Cu-N<sub>2</sub>O<sub>2</sub> sites, yielding readily polarized magnetic moments. Consequently, a spin-ordered phase emerges on the surface of Cu-N<sub>2</sub>O<sub>2</sub>/HCNT under a magnetic field, enhancing formate selectivity. Impressively, Cu-N<sub>2</sub>O<sub>2</sub>/HCNT achieves 93.6 % formate selectivity at −0.80 V vs. RHE under 200 mT. Under an in situ magnetic field, it maintains over 80 % formate selectivity at −175 mA/cm<sup>2</sup> for 100 h. Our findings offer novel insights into single-atom catalyst modification.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 347-355"},"PeriodicalIF":13.1,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678985","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}

引用次数: 0

Recent advances in metallic core–shell nanoparticles for electrocatalysis: synthesis, characterization, and applications 电催化用金属核壳纳米颗粒的合成、表征及应用研究进展

IF 13.1 1区化学

Journal of Energy Chemistry Pub Date : 2025-07-04 DOI: 10.1016/j.jechem.2025.06.057

Xiangyun Xiao , Doufeng Wang , Osama Younis , Xiaolong Zhang , Ahmed F. Al-Hossainy , Cafer T. Yavuz , Xinchun Yang , Hui-Ming Cheng

{"title":"Recent advances in metallic core–shell nanoparticles for electrocatalysis: synthesis, characterization, and applications","authors":"Xiangyun Xiao , Doufeng Wang , Osama Younis , Xiaolong Zhang , Ahmed F. Al-Hossainy , Cafer T. Yavuz , Xinchun Yang , Hui-Ming Cheng","doi":"10.1016/j.jechem.2025.06.057","DOIUrl":"10.1016/j.jechem.2025.06.057","url":null,"abstract":"<div><div>Metallic core–shell nanoparticles (MCSNs) have attracted significant research interest in electrochemical energy conversion owing to their distinctive microstructures and superior catalytic performances. By rationally designing a metallic core with a specific surface (shell), synergistic interactions between the core and the shell, benefiting from the intrinsic strain, ligand, geometric, and ensemble effects, can endow multi-metallic CSNs with highly enhanced activity, selectivity, and stability in electrocatalytic reactions, compared to their monometallic counterparts. In this review, we outline the key breakthroughs—especially in the past 5 years—of MCSNs, focusing on their precise design/synthesis, intrinsic effects arising from core–shell interactions, state-of-the-art characterization techniques, and exceptional performance in critical electrochemical reactions, including water splitting, oxygen reduction reaction (ORR), CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR), N<sub>2</sub>/NO<sub>3</sub><sup>−</sup> reduction reaction (N<sub>2</sub>RR/NO<sub>3</sub>RR), and small organic molecule electrooxidations. We further discuss the ongoing challenges and opportunities for MCSNs, particularly in achieving computationally guided design/atomic-precision synthesis, enabling scalable production, and advancing in situ or operando characterization methods. We hope that the present review will inspire chemists working in this field to develop new MCSNs for sustainable energy applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"110 ","pages":"Pages 227-245"},"PeriodicalIF":13.1,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144663473","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}

引用次数: 0