Mingchen Yang, Xiuyang Zou, Mingzhu Wu, Jiangtao Yu, Xinyu Ma, Yin Hu and Feng Yan
{"title":"Halozincate ionic liquid electrolyte enabled high-temperature dendrite-free Zn metal batteries†","authors":"Mingchen Yang, Xiuyang Zou, Mingzhu Wu, Jiangtao Yu, Xinyu Ma, Yin Hu and Feng Yan","doi":"10.1039/D4EE06146B","DOIUrl":"10.1039/D4EE06146B","url":null,"abstract":"<p >Aqueous Zn metal batteries (ZMBs) are receiving increasing attention due to their safety, cost-effectiveness, and scalability. However, aqueous ZMBs suffer from the hydrogen evolution reaction (HER), dendrite growth, and intrinsic volatility of electrolytes at high temperatures, hindering their practical application in mining/drilling, industrial manufacturing, and aerospace. Here, we introduce an anhydrous electrolyte design by using halozincate ionic liquid electrolyte (HZLE) to achieve dendrite-free Zn anode chemistry and facilitate high-temperature ZMBs. The halozincate solvation structure in HZLE pulls out a coordination channel for fast Zn<small><sup>2+</sup></small> transport and enables high reversible deposition/dissolution of the Zn anode. The Zn‖Ti cells show uniform Zn deposition with an average Zn plating/stripping Coulombic efficiency (CE) of 99.99%. As a result, Na<small><sub>3</sub></small>V<small><sub>2</sub></small>(PO<small><sub>4</sub></small>)<small><sub>3</sub></small>‖Zn batteries exhibit high CE exceeding 99.81% at 25 °C and can sustain 1000 deep cycles at 80 °C. This HZLE design offers an opportunity for alkali–metal–ion batteries to operate at high temperatures.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 7","pages":" 3365-3375"},"PeriodicalIF":32.4,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Feng Wang, Lian Chen, Jiaqi Wei, Caozheng Diao, Fan Li, Congcong Du, Zhengshuai Bai, Yanyan Zhang, Oleksandr I. Malyi, Xiaodong Chen, Yuxin Tang, Xiaojun Bao
{"title":"Pushing slope- to plateau-type behavior in hard carbon for sodium-ion batteries via local structure rearrangement","authors":"Feng Wang, Lian Chen, Jiaqi Wei, Caozheng Diao, Fan Li, Congcong Du, Zhengshuai Bai, Yanyan Zhang, Oleksandr I. Malyi, Xiaodong Chen, Yuxin Tang, Xiaojun Bao","doi":"10.1039/d5ee00104h","DOIUrl":"https://doi.org/10.1039/d5ee00104h","url":null,"abstract":"Elucidating the microstructure of hard carbon is essential for uncovering the sodium storage mechanism and constructing state-of-the-art hard carbon anodes for sodium-ion batteries. Guided by understanding the crystallization process and inverse materials design principles, we design hard carbon anodes with different local fragments to understand the correlating microstructure of hard carbon and sodium storage behaviors from the commercialization perspective. The sodiation transformation of hard carbon from slope- to plateau-type is realized via a series of local structure rearrangements, including interlayer distance, average crystallite width of graphitic domains, and defect density. We found that the increase in plateau capacity is mainly related to the transition from critical interlayer distance to average crystallite width of graphitic domains control, and is limited by the closed pore volume of hard carbon. During sodiation, the formation of NaF and Na2O in the slope region, as well as Na2O2 and NaO2 in the plateau region, are always accompanied by the production of Na2CO3. This work provides insights into understanding the sodium storage behavior in hard carbon anodes and defines general structural design principles from the slope- to plateau type of hard carbon.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"51 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495801","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"From Lab-Scale to Industrialization: Atomically M-N-C Catalysts for Oxygen Reduction Reaction","authors":"Tianyou Zhao, Jianjiang Wang, Yanrui Wei, Zechao Zhuang, Yuhai Dou, Jiarui Yang, Wen-Hao Li, Dingsheng Wang","doi":"10.1039/d5ee00074b","DOIUrl":"https://doi.org/10.1039/d5ee00074b","url":null,"abstract":"Atomically M-N-C catalysts have become a prominent research focus in new energy technologies due to their outstanding performance in oxygen reduction reaction. To date, various M-N-C catalysts have been developed as foundational research models for realizing high-efficiency fuel cells. With the help of atomically theoretical research tools, our understanding of the electronic interactions between active sites and microstructures has reached a new level. However, a significant gap remains between theoretical advancements at the laboratory scale and their industrial applications. Therefore, bridging this gap is an urgent need. This review addresses key aspects of M-N-C catalysts by summarizing the construction, characterization, mechanistic research (including probes and density functional theory calculations), machine learning, and high throughput design of active centers at the atomically. The review highlights the critical issues that must be resolved in industrialization and outlines future development directions. With the goal of \"accelerating industrialization through industrial technology,\" this review provides a comprehensive overview and valuable reference for future research.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"68 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495800","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Multi-Stage Collaborative Design of Hierarchical Twisted Hydrogel Electrolytes for Aqueous Zinc-Ion Batteries with High Capacity, Ultralong Stability, and Mechanical Robustness","authors":"Weiyan Zhu, Zhouyue Lei, Peiyi Wu","doi":"10.1039/d5ee00001g","DOIUrl":"https://doi.org/10.1039/d5ee00001g","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) are promising energy storage systems due to their high theoretical capacity, intrinsic safety, and potentially high cycling stability. However, their practical application is hindered by sluggish Zn-ion transfer, parasitic side reactions, and dendrite growth, leading to suboptimal capacity and limited cycle lifespan. Herein, we report a bioinspired design of hierarchical twisted hydrogel electrolytes (HTHEs) by establishing a multi-stage collaborative regulation pathway to address these challenges. The HTHE exhibits a high Zn2+ transference number of 0.9 and a wide electrochemical stability window of 2.61 V, effectively suppressing dendrite formation and enhancing Zn2+ deposition along the Zn (002) plane. Symmetric cells assembled with the HTHE demonstrate exceptional cycling stability across a wide range of current densities, while pouch cells achieve an ultra-long cycle life of nearly 10000 cycles with a high specific capacity of >100 mAh g-1 and 80% capacity retention. Notably, these pouch cells display outstanding flexibility and impact resistance, remaining fully operational under folding and even withstanding extreme mechanical stresses, such as those even crack walnuts. The multi-stage collaborative regulation pathway in the design of high-performance flexible AZIB electrolytes enhances their potential for next-generation energy storage applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"85 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495802","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junkang Zhou, Xinjie Zhou, Hongge Jia, Lijun Tu, Siqi Wu, Xiaomin Xia, Xin Song and Yongqiang Shi
{"title":"20.0% efficiency of ternary organic solar cells enabled by a novel wide band gap polymer guest donor†","authors":"Junkang Zhou, Xinjie Zhou, Hongge Jia, Lijun Tu, Siqi Wu, Xiaomin Xia, Xin Song and Yongqiang Shi","doi":"10.1039/D4EE05848H","DOIUrl":"10.1039/D4EE05848H","url":null,"abstract":"<p >The ternary strategy has emerged as a promising approach to further improve the device performance of organic solar cells (OSCs). Herein, a novel wide bandgap polymer donor <strong>P(BTzE-BDT)</strong> was synthesized and incorporated into the <strong>PM6</strong>:<strong>BTP-eC9</strong> system to fabricate ternary OSCs. <strong>P(BTzE-BDT)</strong> exhibits complementary absorption spectra and excellent compatibility with <strong>PM6</strong>, facilitating the fine-tuning of photon harvesting and the morphology of the ternary blend films. This leads to a simultaneous increase in the short-circuit current density (<em>J</em><small><sub>SC</sub></small>) and fill factor (FF). By promoting intensive molecular packing and reducing domain size, <strong>P(BTzE-BDT)</strong> optimizes the morphology, contributing to improved and well-balanced charge transport, suppressed carrier recombination, and efficient exciton dissociation. Consequently, ternary OSCs with a 5% addition of <strong>P(BTzE-BDT)</strong> exhibit a higher power conversion efficiency (PCE) of 20.0%, compared to 18.8% for the binary system. Furthermore, thick-film devices were fabricated to assess their commercialization potential, achieving a PCE of 18.2% with an active layer thickness of 300 nm, compared to 16.3% for the binary device. This comprehensive study underscores the potential of <strong>P(BTzE-BDT)</strong> as a promising guest molecule for optimizing morphology, which is crucial for achieving high efficiency in OSCs, thereby paving the way for practical commercial applications.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 7","pages":" 3341-3351"},"PeriodicalIF":32.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Integrated Modeling the Transition Pathway of China’s Power System","authors":"Ziheng Zhu, Da Zhang, Xiaoye Zhang, Xiliang Zhang","doi":"10.1039/d5ee00355e","DOIUrl":"https://doi.org/10.1039/d5ee00355e","url":null,"abstract":"Accelerating decarbonization of the power system is at the heart of achieving China’s carbon neutrality goal and mitigating global climate change. However, deploying multi-terawatts of variable renewable energy (VRE) may result in substantial system volatility. Here, using a temporally and spatially resolved model co-optimizing capacity expansion and system operation throughout the full 8,760 hours in a planning year, we show that achieving −550 MtCO2/yr of negative emissions is feasible for China’s power system by 2060 with 6,000 GW of VRE, 5,800 GWh of energy storage, and 850 MtCO2/yr of carbon capture and sequestration (CCS), at the marginal carbon abatement cost of 750–1,100 yuan/tCO2 (about 108–157 $/tCO2). Multi-millions of hectares of land areas are necessary to accommodate the TW-scale installation of solar photovoltaic panels, with restricted land policies resulting in a 3.3% increase in electricity costs. System volatility also surges with higher penetration of VRE, represented by increasing variability in hourly marginal demand cost, necessitating firm resources to ensure capacity adequacy. Although these firm sources can earn higher generation revenues in peak hours, capacity compensation amounts to hundreds of yuan/kW (about tens of $/kW) per year is still needed. Effective planning and policy formulation are essential to support China’s decarbonization effort for its power sector.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"68 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shengwen Zou, Jingjing Zhang, Yi Xin, Jinlong Jin, Guangxin Liu, Xiaojun Yan and Jianmei Huang
{"title":"Moisture-inhibited deprotonation at the buried interface enables efficient perovskite solar cells with a high fill factor of over 86%†","authors":"Shengwen Zou, Jingjing Zhang, Yi Xin, Jinlong Jin, Guangxin Liu, Xiaojun Yan and Jianmei Huang","doi":"10.1039/D4EE04555F","DOIUrl":"10.1039/D4EE04555F","url":null,"abstract":"<p >SnO<small><sub>2</sub></small> is one of the best electron-transport materials for perovskite solar cells (PSCs). However, the limited interfacial contact and the reaction occurring at the buried interface between the perovskite and SnO<small><sub>2</sub></small> reduce their performance. Herein, we revealed a strong deprotonation reaction of formamidinium cation that occurred at the buried interface during perovskite growth under a nitrogen atmosphere. In contrast, this reaction was considerably inhibited by moisture when the perovskite was grown under an ambient atmosphere (Amb-perovskite). Thus, defects at the buried interface of the Amb-perovskite were reduced, considerably suppressing the non-radiative recombination. Amb-PSC resulted in an efficiency of 25.69%, with an ultra-high fill factor of 86.21% and enhanced operational stability without decay after more than 1000 h under continuous 1-sun illumination. This work provides an efficient strategy for perovskite film annealing under an ambient atmosphere to minimise the buried interface loss. Its scaling-up potential and easy-processibility make it a promising strategy for low-cost large-scale manufacturing of PSCs.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 7","pages":" 3385-3394"},"PeriodicalIF":32.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486556","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Do-Wan Kim, Hyeonwoo Mun, Yeonghun Kang, Weon-Guk Kim, Dahye Ahn, Seong-Yun Yun, Jeong-A Han, Do Hoon Lee, Taegoon Lee, Kihoon Jeong, Jihan Kim, Sung Gap Im, Yang-Kyu Choi
{"title":"Synthesis of stretchable triboelectric material with strain-compensating ability using gradient interpenetrating polymer networks","authors":"Do-Wan Kim, Hyeonwoo Mun, Yeonghun Kang, Weon-Guk Kim, Dahye Ahn, Seong-Yun Yun, Jeong-A Han, Do Hoon Lee, Taegoon Lee, Kihoon Jeong, Jihan Kim, Sung Gap Im, Yang-Kyu Choi","doi":"10.1039/d4ee03110e","DOIUrl":"https://doi.org/10.1039/d4ee03110e","url":null,"abstract":"Unlike conventional rigid triboelectric nanogenerators (TENGs), elastic TENGs are considered attractive for energy harvesting and sensing applications in mechanically harsh conditions. However, the practicality of elastic TENGs has been limited by the lack of elastic materials that simultaneously possess the desired mechanical and triboelectric properties. This paper introduces a complementary material synthesis strategy that uses a gradient interpenetrating polymer network (g-IPN) to address this issue. A sub-micron thick g-IPN was formed on a host elastomer (Ecoflex-CNT) that has high contact conformity using a highly chargeable guest polymer (pVP) with a low work function, through initiated chemical vapor deposition (iCVD) process. This complementary material synthesis effectively leveraged only the strengths of each component and resulted in a synergistic enhancement in output performance, with a short-circuit charge density (<em>Q</em><small><sub>SC</sub></small>) and an open-circuit voltage (<em>V</em><small><sub>OC</sub></small>) up to 445 μC m<small><sup>-2</sup></small> and 1335 V, respectively. These values were achieved without affecting bulk mechanical properties of the host elastomer, such as high stretchability and low bulk elastic modulus. Moreover, the depth-directional gradient profile of the g-IPN effectively prevented degradation in output performance under a severely stretched state (up to 100% strain), through a so-called strain-compensating ability. The effectiveness of the g-IPN in three-dimensional (3D)-structured elastic TENGs was successfully demonstrated by applying the g-IPN to a sponge-structured 3D elastic TENG (3D-IPN-TENG), which benefited from the exceptional deposition conformity of the iCVD process. The fabricated 3D-IPN-TENG showed stable operation with a short-circuit volume charge density (<em>Q</em><small><sub>SC,vol</sub></small>) of up to 267.2 mC m<small><sup>-3</sup></small>, which is a record-high value among 3D-structured TENGs that utilize contact electrification (CE) between solids. This work not only overcomes the limitations of existing material strategies for elastic TENGs, but also suggests a new universal material design principle for synthesizing high-performance triboelectric materials.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"90 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486557","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Liu, Xiyu Li, Haeseong Jang, Jianghua Wu, Min Gyu Kim, Xiaoke Xi, Zhanwu Lei, Yuchen Zhang, Yu Deng, Wensheng Yan, Jun Jiang, Shuhong Jiao, Jing-Li Luo and Ruiguo Cao
{"title":"Self-limiting surface leaching stabilizes Ru-based catalysts for acidic water oxidation†","authors":"Yang Liu, Xiyu Li, Haeseong Jang, Jianghua Wu, Min Gyu Kim, Xiaoke Xi, Zhanwu Lei, Yuchen Zhang, Yu Deng, Wensheng Yan, Jun Jiang, Shuhong Jiao, Jing-Li Luo and Ruiguo Cao","doi":"10.1039/D4EE05220J","DOIUrl":"10.1039/D4EE05220J","url":null,"abstract":"<p >Ru-based catalysts are a promising alternative to Ir-based catalysts for the acidic oxygen evolution reaction (OER), but their poor long-term stability remains a significant challenge. Continuous leaching-induced loss of active sites and structural collapse are the primary causes of this instability, severely limiting the practical application of Ru-based catalysts in proton exchange membrane (PEM) electrolyzers. Here, we present a self-limiting surface leaching mechanism that effectively suppresses continuous leaching, thereby significantly prolonging the lifespan of Ru-based catalysts under acidic OER conditions. Specifically, the Ru–Mn solid solution oxide with a hollow shell structure undergoes surface Mn leaching during the initial OER process, resulting in the formation of a Mn-vacancy-rich stable reconstruction layer. This layer effectively inhibits further leaching of both Ru and Mn, thus self-limiting the further degradation of catalysts. As a result, the reconstructed catalyst exhibits an unprecedented durability of up to 2500 h at 10 mA cm<small><sup>−2</sup></small> in 0.5 M H<small><sub>2</sub></small>SO<small><sub>4</sub></small>. This remarkable stability was also validated in PEM electrolyzers, highlighting its practical applicability. <em>Operando</em> synchrotron characterization combined with theoretical calculations reveals that the formation of Mn vacancies increases the demetallation energy of Ru species, thereby suppressing the continuous leaching and enhancing the long-term stability. This work provides valuable insights for designing highly stable catalysts through a self-limiting leaching mechanism.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 7","pages":" 3352-3364"},"PeriodicalIF":32.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ee/d4ee05220j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Boosting the reduction of CO2 and dimethylamine for C–N bonding to synthesize DMF via modulating the electronic structures of indium single atoms","authors":"Jingui Zheng, Shaohan Xu, Lingzhi Sun, Xun Pan, Qihao Xie, Guohua Zhao","doi":"10.1039/d4ee05681g","DOIUrl":"https://doi.org/10.1039/d4ee05681g","url":null,"abstract":"The electrocatalytic reduction of CO<small><sub>2</sub></small> and dimethylamine (HN(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>) for C–N coupling is a promising strategy for synthesizing <em>N</em>,<em>N</em>-dimethylformamide (DMF). However, the generation of suitable coupling intermediates <em>via</em> the dehydrogenation of HN(CH<small><sub>3</sub></small>)<small><sub>2</sub></small> and reduction hydrogenation of CO<small><sub>2</sub></small> is the key challenge for achieving C–N bonding to synthesize DMF. We optimized the electronic structure of HN(CH<small><sub>3</sub></small>)<small><sub>2</sub></small> and CO<small><sub>2</sub></small> for adsorption on indium single atoms by adjusting the coordination structure, thereby promoting the hydrogen transfer from nitrogen of dimethylamine to CO<small><sub>2</sub></small>, which generated the intermediates of *N(CH<small><sub>3</sub></small>)<small><sub>2</sub></small> and *COOH for C–N bonding to synthesize DMF. The yield of DMF synthesized on InN<small><sub>3</sub></small> reached 41.3 μmol L<small><sup>−1</sup></small> h<small><sup>−1</sup></small>, which was about 12 times greater than that of InN<small><sub>4</sub></small> at −0.8 V. <em>In situ</em> technology and DFT calculations jointly demonstrated that compared with InN<small><sub>4</sub></small>, InN<small><sub>3</sub></small> optimized the electron distribution of adsorbed CO<small><sub>2</sub></small> and HN(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>. The electron density of hydrogen on HN(CH<small><sub>3</sub></small>)<small><sub>2</sub></small> decreased, exhibiting its electrophilic properties. In addition, oxygen of CO<small><sub>2</sub></small> accumulated electrons near the dimethylamine end and exhibited strong electron-rich properties, which led to hydrogen transfer from dimethylamine to CO<small><sub>2</sub></small>, generating the species *N(CH<small><sub>3</sub></small>)<small><sub>2</sub></small> and *COOH that are conducive to C–N coupling to synthesize DMF on InN<small><sub>3</sub></small>. This work provides important theoretical guidance for the C–N coupling of CO<small><sub>2</sub></small> and amines.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"50 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477353","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}