Journal of Energy Chemistry最新文献

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Interfacial electron regulation of Fe9Ni9S16/FeS heterostructure confined in N-doped carbon nanotube with enhanced reaction kinetics for efficient Na/Li-Ion storage
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-04-01 DOI: 10.1016/j.jechem.2025.03.041
Shufeng Bo , Junmei Luo , Jung Woo Lee , Kwang Ho Kim
{"title":"Interfacial electron regulation of Fe9Ni9S16/FeS heterostructure confined in N-doped carbon nanotube with enhanced reaction kinetics for efficient Na/Li-Ion storage","authors":"Shufeng Bo ,&nbsp;Junmei Luo ,&nbsp;Jung Woo Lee ,&nbsp;Kwang Ho Kim","doi":"10.1016/j.jechem.2025.03.041","DOIUrl":"10.1016/j.jechem.2025.03.041","url":null,"abstract":"<div><div>Tailoring 1D nanotubes with refined interfacial interactions and optimized adsorption sites presents a highly promising yet challenging strategy for advancing Na/Li-ion batteries (SIBs/LIBs). Herein, the intertwined yardlong bean-like Fe<sub>9</sub>Ni<sub>9</sub>S<sub>16</sub>/FeS heterostructures with sulfur vacancies encapsulated in N-doped carbon nanotubes (3 N-Fe<sub>9</sub>Ni<sub>9</sub>S<sub>16</sub>/FeS-3@CNTs) are controllably synthesized through Fe/Ni-catalyzed pyrolysis of dicyandiamide followed by sulfidation strategies. 1D nanotubes with robust outer walls and internal cavity structures shorten the diffusion paths of ions/electrons and buffer volume expansion and aggregation of active materials. The Fe<sub>9</sub>Ni<sub>9</sub>S<sub>16</sub>/FeS heterostructure provides a powerful driving force for charge transfer by forming built-in electric fields, optimizing ion adsorption, while the Fe<sub>9</sub>Ni<sub>9</sub>S<sub>16</sub> features a wider interlayer spacing that allows for frequent Na<sup>+</sup>/Li<sup>+</sup> insertion and extraction, thereby enhancing the reaction kinetics within the electrode. Driven by these synergistic factors, the 3 N-Fe<sub>9</sub>Ni<sub>9</sub>S<sub>16</sub>/FeS-3@CNTs demonstrates remarkable electrochemical performance, achieving a substantial reversible capacity of up to 682.1mA h g<sup>−1</sup> for SIBs at 0.1 A g<sup>−1</sup> and 782.7 mA h g<sup>−1</sup> for LIBs at 0.5 A g<sup>−1</sup>, alongside exceptional cycling stability in SIBs, maintaining 78.7% of its capacity after 1500 cycles at 1 A g<sup>−1</sup> coupling with the ether-based electrolyte. Employing various electrochemical analyses in conjunction with ex-situ characterization techniques and Density Functional Theory (DFT) calculations, the storage mechanisms and phase transition processes are investigated, elucidating the structure-composition-performance relationships. This work paves the way for a new strategy in designing advanced materials with engineered heterostructures and controllable defects for energy conversion and storage devices.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 459-471"},"PeriodicalIF":13.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143864922","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
Stability of hole-selective self-assembled monolayers in inverted perovskite solar cells
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-31 DOI: 10.1016/j.jechem.2025.03.032
Yiting Zheng, Tingting Niu, Lingfeng Chao, Yingdong Xia, Yonghua Chen
{"title":"Stability of hole-selective self-assembled monolayers in inverted perovskite solar cells","authors":"Yiting Zheng,&nbsp;Tingting Niu,&nbsp;Lingfeng Chao,&nbsp;Yingdong Xia,&nbsp;Yonghua Chen","doi":"10.1016/j.jechem.2025.03.032","DOIUrl":"10.1016/j.jechem.2025.03.032","url":null,"abstract":"<div><div>Inverted p-i-n perovskite solar cells (PSCs) based on self-assembled monolayers (SAMs) as hole-selective layers (HSLs) have produced potential record efficiencies of more than 26% by tuning work function, dipole, and passivation defects. However, the stability of the SAM molecules, the stability of the molecular anchoring conformation, and the impact on the stability of subsequent PSCs have not been clearly elucidated. In this review, we systematically discussed the intrinsic connection between the molecular conformation (including anchoring groups, spacer groups, and terminal groups) and the stability of SAMs. Sequentially, the research progress of SAMs as HSLs in improving the stability of PSCs is summarized, including photostability, thermal stability, ion migration, and residual stress. Finally, we look forward to the shortcomings and possible challenges of using SAMs as HSLs for inverted PSCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 74-86"},"PeriodicalIF":13.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838168","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
Mitigating fast-charging degradation in Ni-rich cathodes via enhancing kinetic-mechanical properties 通过增强动力学-机械特性缓解富镍阴极的快速充电降解现象
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-31 DOI: 10.1016/j.jechem.2025.03.033
Yali Wen , Yuzhi He , Yu Tang , Siyu Chen , Liuqi Wang , Zhiyong Huang , Wei Wang , Xingyu Wang , Xingjun Li , Yang Ren , Qi Liu
{"title":"Mitigating fast-charging degradation in Ni-rich cathodes via enhancing kinetic-mechanical properties","authors":"Yali Wen ,&nbsp;Yuzhi He ,&nbsp;Yu Tang ,&nbsp;Siyu Chen ,&nbsp;Liuqi Wang ,&nbsp;Zhiyong Huang ,&nbsp;Wei Wang ,&nbsp;Xingyu Wang ,&nbsp;Xingjun Li ,&nbsp;Yang Ren ,&nbsp;Qi Liu","doi":"10.1016/j.jechem.2025.03.033","DOIUrl":"10.1016/j.jechem.2025.03.033","url":null,"abstract":"<div><div>Ni-rich cathode materials are essential for enhancing the performance of lithium-ion batteries (LIBs) in electric vehicles (EVs), particularly concerning extreme fast charging (XFC) and durability. While much of studies<!--> <!-->shine<!--> <!-->a<!--> <!-->spotlight<!--> <!-->on Li plating on the anode to improve rate capability, there is a critical lack of studies addressing the combination of kinetic improvements and mechanical strength of cathode materials under XFC conditions. In this work, Mg/Ti co-doped Ni-rich LiNi<sub>0.88</sub>Co<sub>0.09</sub>Mn<sub>0.03</sub>O<sub>2</sub> (MT-NCM) was successfully synthesized to address structural challenges associated with high-rate cycling. The results demonstrate that the stronger Ti–O bond contributes to the enhanced mechanical strength of secondary grains, which effectively alleviates microcrack formation during fast charging. Additionally, the detrimental phase transitions and internal strain as well as parasitic reactions of MT-NCM are significantly suppressed due to the synergistic effect of the dual dopants, ensuring excellent Li-ion transport kinetics compared to pristine NCM (P-NCM). Consequently, MT-NCM achieves remarkable high-rate cycling performance, retaining 88.04% of its initial capacity at 5 C and superior discharge capacity over 175 mA h g<sup>−1</sup> even at 10 C. This work highlights the potential of optimizing the kinetic-mechanical properties of Ni-rich cathodes, providing a viable approach for the development of XFC LIBs with improved durability for EV applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 296-304"},"PeriodicalIF":13.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143847382","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
Data-driven classification and prediction of all-inorganic Cs-Pb-Br perovskite crystal structures
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-31 DOI: 10.1016/j.jechem.2025.03.031
Qi Wang , Maolin Lei , Andrea Cicconardi , Giorgio Divitini
{"title":"Data-driven classification and prediction of all-inorganic Cs-Pb-Br perovskite crystal structures","authors":"Qi Wang ,&nbsp;Maolin Lei ,&nbsp;Andrea Cicconardi ,&nbsp;Giorgio Divitini","doi":"10.1016/j.jechem.2025.03.031","DOIUrl":"10.1016/j.jechem.2025.03.031","url":null,"abstract":"<div><div>All-inorganic perovskites based on cesium-lead-bromine (Cs-Pb-Br) have been a prominent research focus in optoelectronics in recent years. The optimisation and tunability of their macroscopic properties exploit the conformational flexibility, resulting in various crystal structures. Varying synthesis parameters can yield distinct crystal structures from Cs, Pb, and Br precursors, and manually exploring the relationship between these synthesis parameters and the resulting crystal structure is both labour-intensive and time-consuming. Machine learning (ML) can rapidly uncover insights and drive discoveries in chemical synthesis with the support of data, significantly reducing both the cost and development cycle of materials. Here, we gathered synthesis parameters from published literature (220 synthesis runs) and implemented eight distinct ML models, including eXtreme Gradient Boosting (XGB), Decision Tree (DT), Support Vector Machine (SVM), Random Forest (RF), Naïve Bayes (NB), Logistic Regression (LR), Gradient Boosting (GB), and K-Nearest (KN) to classify and predict Cs-Pb-Br crystal structures from given synthesis parameters. Validation accuracy, precision, F1 score, recall, and average area under the curve (AUC) are employed to evaluate these ML models. The XGB model exhibited the best performance, achieving a validation accuracy of 0.841. The trained XGB model was subsequently utilised to predict the structure from 10 experimental runs using a randomised set of parameters, achieving a testing accuracy of 0.8. The results indicate that the Cs/Pb molar ratio, reaction time, and the concentration of organic compounds (ligands) play crucial roles in synthesising various crystal structures of Cs-Pb-Br. This study demonstrates a significant decrease in effort required for experimental procedures and builds a foundational basis for predicting crystal structures from synthesis parameters.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 203-211"},"PeriodicalIF":13.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143843570","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
Modulating electronic structure and hydrogen bond network via asymmetric S–Ru–O interfaces for superior alkaline hydrogen oxidation catalysis
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-31 DOI: 10.1016/j.jechem.2025.03.034
Chenggong Niu , Yi Liu , Shuqing Zhou , Heyang Liu , Linyu Chen , Jingya Guo , Tayirjan Taylor Isimjan , Xiulin Yang
{"title":"Modulating electronic structure and hydrogen bond network via asymmetric S–Ru–O interfaces for superior alkaline hydrogen oxidation catalysis","authors":"Chenggong Niu ,&nbsp;Yi Liu ,&nbsp;Shuqing Zhou ,&nbsp;Heyang Liu ,&nbsp;Linyu Chen ,&nbsp;Jingya Guo ,&nbsp;Tayirjan Taylor Isimjan ,&nbsp;Xiulin Yang","doi":"10.1016/j.jechem.2025.03.034","DOIUrl":"10.1016/j.jechem.2025.03.034","url":null,"abstract":"<div><div>Triggering structural asymmetry can induce charge redistribution and modify electronic structures, which is of great significance for the design of high-performance hydrogen oxidation reaction (HOR) electrocatalysts. Herein, we propose a dual anion-induced strategy to create an innovative RuS<sub>2</sub>-RuO<sub>2</sub> heterostructure featuring abundant S–Ru–O interfaces (RuS<sub>2</sub>-RuO<sub>2</sub>@C). This RuS<sub>2</sub>-RuO<sub>2</sub>@C demonstrates an impressive mass activity of 2.61 mA <span><math><mrow><msubsup><mrow><mi>μ</mi><mi>g</mi></mrow><mrow><mi>R</mi><mi>u</mi></mrow><mrow><mo>-</mo><mn>1</mn></mrow></msubsup></mrow></math></span> and an exchange current density of 2.96 mA cm<sup>−2</sup>, surpassing Pt/C and other comparative samples by over 20 times. Durability assessments confirm the superior stability of RuS<sub>2</sub>-RuO<sub>2</sub>@C, with only minimal performance loss during operation. Density functional theory (DFT) calculations indicate that the asymmetric S–Ru–O configuration optimizes the interfacial electronic structure and shifts the <em>d</em>-band center closer to the Fermi level, effectively reducing the energy barrier of the rate-determining step (RDS) in the alkaline HOR process. Moreover, in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characteristics disclose the formation of a substantial hydrogen bond network at the S–Ru–O interface, which aids in the desorption of H<sub>2</sub>O<sub>ad</sub> and facilitates the vital Volmer step in the HOR pathway.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 9-17"},"PeriodicalIF":13.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143834571","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
Ruthenium catalyst supported on perovskite-type alkaline earth metal-titanates with strong metal-support interaction for ammonia decomposition
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-29 DOI: 10.1016/j.jechem.2025.03.026
Dexing Li , Zhili Yin , Peixian Wang, Ziqing Wang, Qin Wu, Zhong Wei
{"title":"Ruthenium catalyst supported on perovskite-type alkaline earth metal-titanates with strong metal-support interaction for ammonia decomposition","authors":"Dexing Li ,&nbsp;Zhili Yin ,&nbsp;Peixian Wang,&nbsp;Ziqing Wang,&nbsp;Qin Wu,&nbsp;Zhong Wei","doi":"10.1016/j.jechem.2025.03.026","DOIUrl":"10.1016/j.jechem.2025.03.026","url":null,"abstract":"<div><div>Alkaline earth-metal titanates ATiO<sub>3</sub> (A = Ca, Sr, and Ba) with a perovskite-type structure were used as supports for Ru-based catalysts to produce CO<em><sub>x</sub></em>-free H<sub>2</sub> via NH<sub>3</sub> decomposition. The effects of alkaline-earth metals on the physicochemical characteristics and catalytic activities of Ru/ATiO<sub>3</sub> for NH<sub>3</sub> decomposition were investigated using various techniques. The order of Ru/ATiO<sub>3</sub> for NH<sub>3</sub> conversion is Ru/BaTiO<sub>3</sub> &gt; Ru/SrTiO<sub>3</sub> &gt; Ru/CaTiO<sub>3</sub> &gt; Ru/TiO<sub>2</sub> at the identical conditions, with the Ru/BaTiO<sub>3</sub> catalyst demonstrating the highest NH<sub>3</sub> conversion of 77.8% at 450 °C and a gas hourly space velocity of 30,000 mL/g<sub>cat</sub>/h, which is 8.7, 2.1, and 1.3 times of that over Ru/TiO<sub>2</sub>, Ru/CaTiO<sub>3</sub>, and Ru/SrTiO<sub>3</sub>, respectively. The formation of the ATiO<sub>3</sub> phase can enrich the concentration of basic sites and oxygen vacancies compared with TiO<sub>2</sub>, which can induce the presence of strong metal-support interaction (SMSI) through the formation of Ru–O–Ti bonds. This SMSI effect increased the dispersion and electron density of Ru nano-particles on ATiO<sub>3</sub> supports, and the electron-rich Ru nano-particles could weaken the chemisorptive strength of N<sub>2</sub> and H<sub>2</sub> on the Ru/ATiO<sub>3</sub> catalysts, thereby promoting the reaction rate for NH<sub>3</sub> decomposition.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 791-802"},"PeriodicalIF":13.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838548","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
Supramolecular interaction chemistry in polymer electrolytes towards stable lithium metal batteries
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-29 DOI: 10.1016/j.jechem.2025.03.025
Yu Zhao , Tianlu Ma , Liang Hu , Xiuyun Ren , Xiaoqi Sun , Xiaoliang Yu
{"title":"Supramolecular interaction chemistry in polymer electrolytes towards stable lithium metal batteries","authors":"Yu Zhao ,&nbsp;Tianlu Ma ,&nbsp;Liang Hu ,&nbsp;Xiuyun Ren ,&nbsp;Xiaoqi Sun ,&nbsp;Xiaoliang Yu","doi":"10.1016/j.jechem.2025.03.025","DOIUrl":"10.1016/j.jechem.2025.03.025","url":null,"abstract":"<div><div>Developing advanced polymer electrolytes in lithium metal batteries (LMBs) has gained significant attention because of their inherent safety advantages over liquid electrolytes, while still encountering great challenges in mitigating uneven lithium plating/stripping and dendrite growth. Previous efforts primarily focused on passive approaches to mechanically constrain lithium dendrite growth. Recent studies have revealed the significance and effectiveness of regulating supramolecular interactions between polymer chains and other electrolyte components for homogenizing lithium deposition and enhancing the interfacial stability. This report provides a timely critical review to cover recent inspiring advancements in this direction. We first summarize the origins of supramolecular interaction origins, strength-determining factors, and structure–property relationships to establish quantitative correlations between polymer composition and supramolecular interaction properties. Then the recent advances in regulating supramolecular interaction chemistry are comprehensively discussed, focusing on those towards accelerated mass transport and stabilized anode-electrolyte interface. Finally, the remaining challenges are highlighted, and potential future directions in supramolecular interaction regulation of polymer electrolytes are prospected for the practical application of LMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 154-169"},"PeriodicalIF":13.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838173","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
Re-adsorption of leached Cr species during the surface reconstruction of NiFeCr layered double hydroxides enhances the oxygen evolution reaction
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-29 DOI: 10.1016/j.jechem.2025.03.030
Tongtong Luo, Shichao Du, Haisheng Zhang, Yishuo Chang, Zhiyu Ren, Honggang Fu
{"title":"Re-adsorption of leached Cr species during the surface reconstruction of NiFeCr layered double hydroxides enhances the oxygen evolution reaction","authors":"Tongtong Luo,&nbsp;Shichao Du,&nbsp;Haisheng Zhang,&nbsp;Yishuo Chang,&nbsp;Zhiyu Ren,&nbsp;Honggang Fu","doi":"10.1016/j.jechem.2025.03.030","DOIUrl":"10.1016/j.jechem.2025.03.030","url":null,"abstract":"<div><div>Cr leaching is anticipated to extensively advance the activity of Cr-containing catalysts towards the oxygen evolution reaction (OER), but the underlying catalytic enhancement mechanism requires further investigation. Herein, NiFeCr layered double hydroxide (NiFeCr-LDH) is proposed as a proof-of-concept catalyst to elucidate the evolution of Cr species and its enhancement mechanism in OER. The incorporation of Cr(Ⅲ) ions into the lattice of NiFe-LDH is achieved through a meticulously controlled electrodeposition process, which not only promotes Cr leaching but also deepens surface reconstruction. More importantly, experimental and theoretical results demonstrate that protogenetic CrO<sub>4</sub><sup>2−</sup> anions, derived from the oxidation of leached Cr ions, adsorb onto the surface NiFeCr-LDH under the anodic potential to create a CrO<sub>4</sub><sup>2−</sup>-rich electrical double layer (CrO<sub>4</sub><sup>2−</sup>-rich EDL) and function as co-catalyst to trigger OER. CrO<sub>4</sub><sup>2−</sup>-rich EDL integrated with vacancies balances the Gibbs free energies of the reconstructed NiFeCr-LDH for oxygen-containing intermediates, resulting in an exceptionally low overpotential of 286 mV at 500 mA cm<sup>−2</sup>, which outperforms most state-of-the-art metallic catalysts. Additionally, the anion exchange membrane water electrolysis system assembled with NiFeCr-LDH and Pt/C demonstrates 1000-h stability at a current density of 1.0 A cm<sup>−2</sup> under a voltage of 1.74 V (at 70 °C), highlighting its promising potential for practical, large-scale and sustainable applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 53-62"},"PeriodicalIF":13.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838167","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
New insights into the long-range interaction mechanism of nitrogen reduction
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-29 DOI: 10.1016/j.jechem.2025.03.024
Yumeng Cheng , Wei Chen , Cheng He , Wenxue Zhang
{"title":"New insights into the long-range interaction mechanism of nitrogen reduction","authors":"Yumeng Cheng ,&nbsp;Wei Chen ,&nbsp;Cheng He ,&nbsp;Wenxue Zhang","doi":"10.1016/j.jechem.2025.03.024","DOIUrl":"10.1016/j.jechem.2025.03.024","url":null,"abstract":"<div><div>Catalysts with asymmetric coordination exhibit excellent electrocatalytic activity due to changes in the active sites, which affect the arrangement of reactants and catalytic activity/selectivity. Hence, the exploration of the inherent characteristics of active sites within diverse coordination environments holds great significance for the experimental design of catalytic structures. Single-atom catalysts (SACs) characterized by high coordination with four carbons (26 candidates) and low coordination with dinitrogen (27 candidates) are constructed using nitrogen-doped graphdiyne derivatives (NGDY) as the substrate. Additionally, 5 species of dual-atom catalysts (DACs) with coexistence of both high and low coordination sites are also developed and their nitrogen reduction reaction (NRR) activities are systematically investigated by density functional theory. The results indicate that metals with low coordination exhibit superior catalytic performance, such as Mo<sup>L</sup>-NGDY (<em>U</em><sub>L</sub> =  −0.30 V) and Nb<sup>L</sup>-NGDY (<em>U</em><sub>L</sub> =  −0.32 V). Furthermore, machine learning (ML) methods have deeply analyzed and elucidated the primary intrinsic characteristics that influence catalytic performance. These results not only unveil the underlying mechanisms behind the exceptional catalytic performance exhibited by low-coordination metal atoms, but also provide relevant and significant descriptors. More importantly, based on an investigation of the catalytic activity of a series of DACs, the “buffer and low-coordination accumulate” asymmetric coordination mechanism is proposed to unveil the long-range interactions between low and high coordination atoms. Due to this remote communication, MoNb-NGDY (<em>U</em><sub>L</sub> =  −0.09/−0.37 V) exhibits the best NRR activity. This mechanism provides valuable insights into the origin of long-range bipartite interactions and inspires the design and synthesis of NRR catalysts with different coordination environments.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"106 ","pages":"Pages 842-851"},"PeriodicalIF":13.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838554","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
A lignin-based polyelectrolyte with fast 3D Li+ transportation network
IF 13.1 1区 化学
Journal of Energy Chemistry Pub Date : 2025-03-29 DOI: 10.1016/j.jechem.2025.03.029
Pengfei Sun , Yeqiang Zhang , Chengdong Fang, Jinji Lan, Yanping Chen, Liubin Feng, Jiajia Chen
{"title":"A lignin-based polyelectrolyte with fast 3D Li+ transportation network","authors":"Pengfei Sun ,&nbsp;Yeqiang Zhang ,&nbsp;Chengdong Fang,&nbsp;Jinji Lan,&nbsp;Yanping Chen,&nbsp;Liubin Feng,&nbsp;Jiajia Chen","doi":"10.1016/j.jechem.2025.03.029","DOIUrl":"10.1016/j.jechem.2025.03.029","url":null,"abstract":"<div><div>In this work, we have developed a lignin-derived polymer electrolyte (LSELi), which demonstrates exceptional ionic conductivity of 1.6 × 10<sup>−3</sup> S cm<sup>−1</sup> and a high cation transference number of 0.57 at 25 °C. Time of flight secondary ion mass spectrometry (TOF-SIMS) analysis shows that the large-size 1-ethyl-3-methylimidazolium cations (EMIM<sup>+</sup>) can induce the aggregation of the anionic segments in lignosulfonate to reconstruct the three-dimensional (3D) spatial structure of polyelectrolyte, thereby forming a fluent Li<sup>+</sup> transport 3D network. Dielectric loss spectroscopy further reveals that within this transport network, Li<sup>+</sup> transport is decoupled from the relaxation of lignosulfonate chain segments, exhibiting characteristics of rapid Li<sup>+</sup> transport. Furthermore, in-situ distribution of relaxation times analysis indicates that a stable solid electrolyte interface layer is formed at the Li plating interface with LSELi, optimizing the Li plating interface and exhibiting low charge transfer impedance and stable Li plating and stripping. Thus, a substantially prolonged cycling stability and reversibility are obtained in the Li||LSELi||Li battery at 25 °C (1800 h at 0.1 mA cm<sup>−2</sup>, 0.1 mAh cm<sup>−2</sup>). At 25 °C, the Li||LSELi||LiFePO<sub>4</sub> cell shows 132 mAh g<sup>−1</sup> of capacity with 92.7% of retention over 120 cycles at 0.1 mA cm<sup>−2</sup>.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"107 ","pages":"Pages 114-121"},"PeriodicalIF":13.1,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143838170","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
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