{"title":"Additive-Free Ti3C2Tx MXene/Carbon Nanotube Aqueous Inks Enable Energy Density Enriched 3D-Printed Flexible Micro-Supercapacitors for Modular Self-Powered Systems","authors":"Yunlong Zhou, Jing Li, Haiyang Fu, Na Li, Simin Chai, Tengfei Duan, Lijian Xu, Zheng-Jun Wang, Jianxiong Xu","doi":"10.1002/cey2.698","DOIUrl":"https://doi.org/10.1002/cey2.698","url":null,"abstract":"<p>3D-printed Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene-based interdigital micro-supercapacitors (MSCs) have great potential as energy supply devices in the field of microelectronics due to their short ion diffusion path, high conductivity, excellent pseudocapacitance, and fast charging capabilities. However, searching for eco-friendly aqueous Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene-based inks without additives and preventing severe restack of MXene nanosheets in high-concentration inks are significantly challenging. This study develops an additive-free, highly printable, viscosity adjustable, and environmentally friendly MXene/carbon nanotube (CNT) hybrid aqueous inks, in which the CNT can not only adjust the viscosity of Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene inks but also widen the interlayer spacing of adjacent Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene nanosheets effectively. The optimized MXene/CNT composite inks are successfully adopted to construct various configurations of MSCs with remarkable shape fidelity and geometric accuracy, together with enhanced surface area accessibility for electrons and ions diffusion. As a result, the constructed interdigital symmetrical MSCs demonstrate outstanding areal capacitance (1249.3 mF cm<sup>−2</sup>), superior energy density (111 μWh cm<sup>−2</sup> at 0.4 mW cm<sup>−2</sup>), and high power density (8 mW cm<sup>−2</sup> at 47.1 μWh cm<sup>−2</sup>). Furthermore, a self-powered modular system of solar cells integrated with MXene/CNT-MSCs and pressure sensors is successfully tailored, simultaneously achieving efficient solar energy collection and real-time human activities monitoring. This work offers insight into the understanding of the role of CNTs in MXene/CNT ink. Moreover, it provides a new approach for preparing environmentally friendly MXene-based inks for the 3D printing of high-performance MSCs, contributing to the development of miniaturized, flexible, and self-powered printable electronic microsystems.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 4","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.698","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143883848","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}
Carbon EnergyPub Date : 2025-03-20DOI: 10.1002/cey2.708
Wei Li, Ying Xu, Guanhua Wang, Ting Xu, Kui Wang, Shangru Zhai, Chuanling Si
{"title":"Sustainable Carbon-Based Catalyst Materials Derived From Lignocellulosic Biomass for Energy Storage and Conversion: Atomic Modulation and Properties Improvement","authors":"Wei Li, Ying Xu, Guanhua Wang, Ting Xu, Kui Wang, Shangru Zhai, Chuanling Si","doi":"10.1002/cey2.708","DOIUrl":"https://doi.org/10.1002/cey2.708","url":null,"abstract":"<p>Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components, various dimensions, high carbon content, and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently. Due to the catalytic deficiency of neutral carbon atoms, the usage of single lignocellulosic-based carbon materials in electrocatalysis involving energy storage and conversion presents unsatisfactory applicability. However, atomic-level modulation of lignocellulose-based carbon materials can optimize the electronic structures, charge separation, transfer processes, and so forth, which results in substantially enhanced electrocatalytic performance of carbon-based catalysts. This paper reviews the recent advances in the rational design of lignocellulosic-based carbon materials as electrocatalysts from an atomic-level perspective, such as self/external heteroatom doping and metal modification. Then, through systematic discussion of the design principles and reaction mechanisms of the catalysts, the applications of the prepared lignocellulosic-based catalysts in rechargeable batteries and electrocatalysis are reviewed. Finally, the challenges in improving the catalytic performance of lignocellulosic-based carbon materials as electrocatalysts and the prospects in diverse applications are reviewed. This review contributes to the synthesis strategy of lignocellulose-based carbon electrocatalysts via atomic-level modulation, which in turn promotes the lignocellulose valorization for energy storage and conversion.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.708","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171384","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}
Carbon EnergyPub Date : 2025-03-20DOI: 10.1002/cey2.710
Matteo Pitaro, Lorenzo Di Mario, Jacopo Pinna, Diego A. Acevedo-Guzmán, Marios Neophytou, Mindaugas Kirkus, Thomas D. Anthopoulos, Giuseppe Portale, Petra Rudolf, Maria Antonietta Loi
{"title":"Bulk Defects Passivation of Tin Halide Perovskite by Tin Thiocyanate","authors":"Matteo Pitaro, Lorenzo Di Mario, Jacopo Pinna, Diego A. Acevedo-Guzmán, Marios Neophytou, Mindaugas Kirkus, Thomas D. Anthopoulos, Giuseppe Portale, Petra Rudolf, Maria Antonietta Loi","doi":"10.1002/cey2.710","DOIUrl":"https://doi.org/10.1002/cey2.710","url":null,"abstract":"<p>Despite the rapid efficiency increase, tin halide perovskite solar cells are significantly behind their lead-based counterpart, with the highest reported efficiency of 15.38%. The main reason for this large difference is attributed to the instability of Sn<sup>2+</sup>, which easily oxidizes to Sn<sup>4+</sup>, creating Sn vacancies and increasing the open-circuit voltage loss. In this work, we implemented tin thiocyanate (Sn(SCN)<sub>2</sub>) as an additive for passivating the bulk defects of a germanium-doped tin halide perovskite film. Adding Sn<sup>2+</sup> and SCN<sup>−</sup> ions reduces the Sn and iodine vacancies, limiting non-radiative recombination and favoring longer charge-carrier dynamics. Moreover, the addition of Sn(SCN)<sub>2</sub> induces a higher film crystallinity and preferential orientation of the (l00) planes parallel to the substrate. The passivated devices showed improved photovoltaic parameters with the best open-circuit voltage of 0.716 V and the best efficiency of 12.22%, compared to 0.647 V and 10.2% for the reference device. In addition, the passivated solar cell retains 88.7% of its initial efficiency after 80 min of illumination under 100 mW cm<sup>-2</sup> and is substantially better than the control device, which reaches 82.6% of its initial power conversion efficiency only after 30 min. This work demonstrates the passivation potential of tin-based additives, which combined with different counterions give a relatively large space of choices for passivation of Sn-based perovskites.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 6","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.710","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514713","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}
Carbon EnergyPub Date : 2025-03-19DOI: 10.1002/cey2.720
Joo-Won Lee, Haleem Ud Din, Taehun Im, Chang-Kyu Hwang, Jong Min Kim, Jung-Hoon Lee, Sohee Jeong
{"title":"Coordination Tailoring of Pt Single-Atom Catalysts at Room Temperature and Their Exceptional Performance in Hydrogen Evolution Reaction","authors":"Joo-Won Lee, Haleem Ud Din, Taehun Im, Chang-Kyu Hwang, Jong Min Kim, Jung-Hoon Lee, Sohee Jeong","doi":"10.1002/cey2.720","DOIUrl":"https://doi.org/10.1002/cey2.720","url":null,"abstract":"<p>Single-atom catalysts (SACs) have garnered interest in designing their ligand environments, facilitating the modification of single catalytic sites toward high activity and selectivity. Despite various synthetic approaches, it remains challenging to achieve a catalytically favorable coordination structure simultaneously with the feasible formation of SACs at low temperatures. Here, a new type of coordination structure for Pt SACs is introduced to offer a highly efficient hydrogen evolution reaction (HER) catalyst, where Pt SACs are readily fabricated by atomically confining PtCl<sub>2</sub> on chemically driven NO<sub>2</sub> sites in two-dimensional nitrogen-doped carbon nanosheets at room temperature. The resultant Pt SACs form the NO<sub>2</sub>–Pt–Cl<sub>2</sub> coordination structure with an atomic dispersion, as revealed by X-ray spectroscopy and transmission electron microscopy investigations. Moreover, our first-principles density functional theory (DFT) calculations show strong interactions in the coordination by computing the binding energy and charge density difference between PtCl<sub>2</sub> and NO<sub>2</sub>. Pt SACs, established on the NO<sub>2</sub>-functionalized carbon support, demonstrate the onset potential of 25 mV, Tafel slope of 40 mV dec<sup>−1</sup>, and high specific activity of 1.35 A mg<sub>Pt</sub><sup>−1</sup>. Importantly, the Pt SACs also exhibit long-term stability up to 110 h, which is a significant advance in the field of single-atom Pt catalysts. The newly developed coordination structure of Pt SACs features a single Pt active center, providing hydrogen binding ability comparable to that of Pt(111), enhanced long-term durability due to strong metal-support interactions, and the advantage of room-temperature fabrication.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.720","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171191","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}
Carbon EnergyPub Date : 2025-03-19DOI: 10.1002/cey2.713
Guilai Zhang, Hong Gao, Dingyi Zhang, Jun Xiao, Limeng Sun, Jiayi Li, Congcong Li, Yiwen Sun, Xinyao Yuan, Peng Huang, Yi Xu, Xin Guo, Yufei Zhao, Yong Wang, Yao Xiao, Guoxiu Wang, Hao Liu
{"title":"Transformative Catalytic Carbon Conversion Enabling Superior Graphitization and Nanopore Engineering in Hard Carbon Anodes for Sodium-Ion Batteries","authors":"Guilai Zhang, Hong Gao, Dingyi Zhang, Jun Xiao, Limeng Sun, Jiayi Li, Congcong Li, Yiwen Sun, Xinyao Yuan, Peng Huang, Yi Xu, Xin Guo, Yufei Zhao, Yong Wang, Yao Xiao, Guoxiu Wang, Hao Liu","doi":"10.1002/cey2.713","DOIUrl":"https://doi.org/10.1002/cey2.713","url":null,"abstract":"<p>Hard carbons are promising anode materials for sodium-ion batteries (SIBs), but they face challenges in balancing rate capability, specific capacity, and initial Coulombic efficiency (ICE). Direct pyrolysis of the precursor often fails to create a suitable structure for sodium-ion storage. Molecular-level control of graphitization with open channels for Na<sup>+</sup> ions is crucial for high-performance hard carbon, whereas closed pores play a key role in improving the low-voltage (< 0.1 V) plateau capacity of hard carbon anodes for SIBs. However, creation of these closed pores presents significant challenges. This work proposes a zinc gluconate-assisted catalytic carbonization strategy to regulate graphitization and create numerous nanopores simultaneously. As the temperature increases, trace amounts of zinc remain as single atoms in the hard carbon, featuring a uniform coordination structure. This mitigates the risk of electrochemically irreversible sites and enhances sodium-ion transport rates. The resulting hard carbon shows an excellent reversible capacity of 348.5 mAh g<sup>−1</sup> at 30 mA g<sup>−1</sup> and a high ICE of 92.84%. Furthermore, a sodium storage mechanism involving “adsorption–intercalation–pore filling” is elucidated, providing insights into the pore structure and dynamic pore-filling process.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 6","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.713","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514791","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":"Uncovering the Critical Role of Ni on Surface Lattice Stability in Anionic Redox Active Li1.2Ni0.2Mn0.6O2","authors":"Peirong Li, Yande Li, Qi Liang, Yize Niu, Shun Zheng, Zengqing Zhuo, Yunhong Luo, Bocheng Liang, Dong Yang, Jixiang Yin, Supeng Chen, Wanneng Ye, Yuanyuan Pan, Qinghao Li, Pengfei Yu, Xiaosong Liu, Qiang Li","doi":"10.1002/cey2.699","DOIUrl":"https://doi.org/10.1002/cey2.699","url":null,"abstract":"<p>Anionic redox reaction (ARR) can provide extra capacity beyond transition metal (TM) redox in lithium-rich TM oxide cathodes. Practical ARR application is much hindered by the structure instability, particularly at the surface. Oxygen release has been widely accepted as the ringleader of surficial structure instability. However, the role of TM in surface stability has been much overlooked, not to mention its interplay with oxygen release. Herein, TM dissolution and oxygen release are comparatively investigated in Li<sub>1.2</sub>Ni<sub>0.2</sub>Mn<sub>0.6</sub>O<sub>2</sub>. Ni is verified to detach from the lattice counter-intuitively despite the overwhelming stoichiometry of Mn, facilitating subsequent oxygen release of the ARR process. Intriguingly, surface reorganization occurs following regulated Ni dissolution, enabling the stabilization of the surface and elimination of oxygen release in turn. Accordingly, a novel optimization strategy is proposed by adding a relaxation step at 4.50 V within the first cycle procedure. Battery performance can be effectively improved, with voltage decay suppressed from 3.44 mV/cycle to 1.60 mV/cycle, and cycle stability improved from 66.77% to 90.01% after 100 cycles. This work provides new perspectives for clarifying ARR surface instability and guidance for optimizing ARR performance.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 6","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.699","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514792","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}
Carbon EnergyPub Date : 2025-03-12DOI: 10.1002/cey2.697
Yuzhen Qian, Long Su, Hongyue Jing, Chunxiao Chai, Fengjin Xie, Xiaoyong Qiu, Jingcheng Hao
{"title":"Extended Electrochemical Window Via Interfacial Microdomain Regulation by a Bicontinuous Microemulsion-Based Heterogel Electrolyte","authors":"Yuzhen Qian, Long Su, Hongyue Jing, Chunxiao Chai, Fengjin Xie, Xiaoyong Qiu, Jingcheng Hao","doi":"10.1002/cey2.697","DOIUrl":"https://doi.org/10.1002/cey2.697","url":null,"abstract":"<p>Regulating the freedom and distribution of H<sub>2</sub>O molecules has become the decisive factor in enlarging the electrochemical stability window (ESW) of aqueous electrolytes. Compared with the water in a bulk electrolyte, H<sub>2</sub>O molecules at the electrode–electrolyte interface tend to directly split under bias potential. Therefore, the composition and properties of the interfacial microenvironment are the crux for optimizing ESW. Herein, we developed a heterogel electrolyte with wide ESW (4.88 V) and satisfactory ionic conductivity (4.4 mS/cm) inspired by the bicontinuous architecture and surfactant self-assembly behavior in the ionic liquid microemulsion-based template. This electrolyte was capable of expanding the ESW through the dynamic oil/water/electrode interface ternary structure, which enriched the oil phase and assembled the hydrophobic surfactant tails at the interface to prevent H<sub>2</sub>O molecules from approaching the electrode surface. Moreover, the surfactant Tween 20 and polymer network effectively suppressed the activity of H<sub>2</sub>O molecules through H-bond interactions, which was beneficial in expanding the operating voltage range and improving the temperature tolerance. The prepared gel electrolyte demonstrated unparalleled adaptability in various aqueous lithium-based energy storage devices. Notably, the lithium-ion capacitor showed an extended operating voltage of 2.2 V and could provide a high power density of 1350.36 W/kg at an energy density of 6 Wh/kg. It maintained normal power output even in the challenging harsh environment, which enabled 11,000 uninterrupted charge–discharge cycles at 0°C. This work focuses on the regulation of the interfacial microdomain and the restriction of the degree of freedom of H<sub>2</sub>O molecules to boost the ESW of aqueous electrolytes, providing a promising strategy for the advancement of energy storage technologies.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.697","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171282","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}
Carbon EnergyPub Date : 2025-03-12DOI: 10.1002/cey2.689
Vaskuri C. S. Theja, Vaithinathan Karthikeyan, Sanjib Nayak, Gopalan Saianand, Vellaisamy A. L. Roy
{"title":"Tellurium-Free, Sustainable Thermoelectric Device for Mid-Temperature Waste Heat Recovery","authors":"Vaskuri C. S. Theja, Vaithinathan Karthikeyan, Sanjib Nayak, Gopalan Saianand, Vellaisamy A. L. Roy","doi":"10.1002/cey2.689","DOIUrl":"https://doi.org/10.1002/cey2.689","url":null,"abstract":"<p>Famatinite (Cu<sub>3</sub>SbS<sub>4</sub>, <i>p</i>-type) and chalcopyrite (CuFeS<sub>2</sub>, <i>n</i>-type) are well-recognized sustainable minerals with good intermediate-temperature thermoelectric performance. In this article, we utilize the inherent thermoelectric properties of these compounds to demonstrate real-time operational performance as a coupled thermoelectric generator (TEG) for waste heat recovery applications. First, we synthesized the polycrystalline and nano-grained famatinite and chalcopyrite materials with high purity through a sustainable synthesis process of mechanical alloying followed by hot pressing. A maximum output power of ~5 mW by the developed TEG was demonstrated while harvesting from a waste heat source of 723 K. Furthermore, the TEG performance via computational simulations for varied thermal gradients was validated. Our results highlight the sustainable development of thermoelectric power generator from earth-abundant minerals having strong stability and capacity to convert waste heat to electricity, which opens a new direction for fabricating a low-cost TEG for intermediate-temperature applications.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.689","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171284","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":"LiZn/LiAlO2/Li2O-Derived Chemical Confinement Enabling Hierarchical and Oriented Li Plating/Stripping","authors":"Huaming Qian, Xifei Li, Qinchuan Chen, Jingjing Wang, Xiaohua Pu, Wei Xiao, Yanyan Cao, Mengxin Bai, Wenbin Li, Zhengdong Ma, Guiqiang Cao, Ruixian Duan, Gaini Zhang, Kaihua Xu, Kun Zhang, Wei Yan, Jiujun Zhang","doi":"10.1002/cey2.714","DOIUrl":"https://doi.org/10.1002/cey2.714","url":null,"abstract":"<p>ZnO with good lithiophilicity has widely been employed to modify the lithiophobic substrates and facilitate uniform lithium (Li) deposition. The overpotential of ZnO-derived Li anode during cycling depends on the lithiophilicity of both LiZn and Li<sub>2</sub>O products upon lithiation of ZnO. However, the striking differences in the lithiophilicity between Li<sub>2</sub>O and LiZn would result in a high overpotential during cycling. In this research, the Al<sub>2</sub>O<sub>3</sub>/<i>n</i>ZnO (<i>n</i> ≥ 1) hybrid layers were precisely fabricated by atomic layer deposition (ALD) to regulate the lithiophilicity of ZnO phase and Li<sub>2</sub>O/LiZn configuration—determining the actual Li loading amount and Li plating/stripping processes. Theoretically, the Li adsorption energy (<i>E</i><sub>a</sub>) values of LiZn and Li<sub>2</sub>O in the LiZn/Li<sub>2</sub>O configuration are separately predicted as −2.789 and −3.447 eV. In comparison, the <i>E</i><sub>a</sub> values of LiZn, LiAlO<sub>2,</sub> and Li<sub>2</sub>O in the LiZn/LiAlO<sub>2</sub>/Li<sub>2</sub>O configuration upon lithiation of Al<sub>2</sub>O<sub>3</sub>/8ZnO layer are calculated as −2.899, −3.089, and −3.208 eV, respectively. Importantly, a novel introduction of LiAlO<sub>2</sub> into the LiZn/Li<sub>2</sub>O configuration could enable the hierarchical Li plating/stripping and reduce the overpotentials during cycling. Consequently, the Al<sub>2</sub>O<sub>3</sub>/8ZnO-derived hybrid Li-metal anode could exhibit electrochemical performances superior to these of ZnO-derived Li anode in both symmetrical and full cells paired with a LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> (NCM622) cathode.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.714","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171285","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":"Interface Engineering Toward Surface-Activated Catalysts for Advanced Li–CO2 Batteries","authors":"Yanze Song, Bingyi Lu, Zhiwen Min, Haotian Qu, Yingqi Liu, Rui Mao, Yanli Chen, Yuanmiao Sun, Guangmin Zhou","doi":"10.1002/cey2.692","DOIUrl":"https://doi.org/10.1002/cey2.692","url":null,"abstract":"<p>Lithium–carbon dioxide (Li–CO<sub>2</sub>) batteries with high theoretical energy density are regarded as promising energy storage system toward carbon neutrality. However, bidirectional catalysts design for improving the sluggish CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR)/CO<sub>2</sub> evolution reaction (CO<sub>2</sub>ER) kinetics remains a huge challenge. In this work, an advanced catalyst with fast-interfacial charge transfer was subtly synthesized through element segregation, which significantly improves the electrocatalytic activity for both CO<sub>2</sub>RR and CO<sub>2</sub>ER. Theoretical calculations and characterization analysis demonstrate local charge redistribution at the constructed interface, which leads to optimized binding affinity towards reactants and preferred Li<sub>2</sub>CO<sub>3</sub> decomposition behavior, enabling excellent catalytic activity during CO<sub>2</sub> redox. Benefiting from the enhanced charge transfer ability, the designed highly efficient catalyst with dual active centers and large exposed catalytic area can maintain an ultra-small voltage gap of 0.33 V and high energy efficiency of 90.2%. This work provides an attractive strategy to construct robust catalysts by interface engineering, which could inspire further design of superior bidirectional catalysts for Li–CO<sub>2</sub> batteries.</p>","PeriodicalId":33706,"journal":{"name":"Carbon Energy","volume":"7 5","pages":""},"PeriodicalIF":19.5,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cey2.692","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144171283","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}