{"title":"Effects of Rattling Behavior of K and Cd Atoms along Different Directions in Anisotropic KCdAs on Lattice Thermal Transport and Thermoelectric Properties","authors":"Yue Wang, Yinchang Zhao, Jun Ni, Zhenhong Dai","doi":"10.1002/eem2.12764","DOIUrl":"10.1002/eem2.12764","url":null,"abstract":"<p>We employ advanced first principles methodology, merging self-consistent phonon theory and the Boltzmann transport equation, to comprehensively explore the thermal transport and thermoelectric properties of KCdAs. Notably, the study accounts for the impact of quartic anharmonicity on phonon group velocities in the pursuit of lattice thermal conductivity and investigates 3ph and 4ph scattering processes on phonon lifetimes. Through various methodologies, including examining atomic vibrational modes and analyzing 3ph and 4ph scattering processes, the article unveils microphysical mechanisms contributing to the low κ<sub>L</sub> within KCdAs. Key features include significant anisotropy in Cd atoms, pronounced anharmonicity in K atoms, and relative vibrations in non-equivalent As atomic layers. Cd atoms, situated between As layers, exhibit rattling modes and strong lattice anharmonicity, contributing to the observed low κ<sub>L</sub>. Remarkably flat bands near the valence band maximum translate into high PF, aligning with ultralow κ<sub>L</sub> for exceptional thermoelectric performance. Under optimal temperature and carrier concentration doping, outstanding <i>ZT</i> values are achieved: 4.25 (<i>a</i>(<i>b</i>)-axis, p-type, 3 × 10<sup>19</sup> cm<sup>−3</sup>, 500 K), 0.90 (<i>c</i>-axis, p-type, 5 × 10<sup>20</sup> cm<sup>−3</sup>, 700 K), 1.61 (<i>a</i>(<i>b</i>)-axis, n-type, 2 × 10<sup>18</sup> cm<sup>−3</sup>, 700 K), and 3.06 (<i>c</i>-axis, n-type, 9 × 10<sup>17</sup> cm<sup>−3</sup>, 700 K).</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12764","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141173040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yanqi Yuan, Kun Wang, Boan Zhong, Dongkun Yu, Fei Ye, Jing Liu, Joydeep Dutta, Peng Zhang
{"title":"MOF-Derived Iron-Cobalt Phosphide Nanoframe as Bifunctional Electrocatalysts for Overall Water Splitting","authors":"Yanqi Yuan, Kun Wang, Boan Zhong, Dongkun Yu, Fei Ye, Jing Liu, Joydeep Dutta, Peng Zhang","doi":"10.1002/eem2.12747","DOIUrl":"10.1002/eem2.12747","url":null,"abstract":"<p>Transition metal phosphides (TMPs) have emerged as an alternative to precious metals as efficient and low-cost catalysts for water electrolysis. Elemental doping and morphology control are effective approaches to further improve the performance of TMPs. Herein, Fe-doped CoP nanoframes (Fe-CoP NFs) with specific open cage configuration were designed and synthesized. The unique nano-framework structured Fe-CoP material shows overpotentials of only 255 and 122 mV at 10 mA cm<sup>−2</sup> for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively, overwhelming most transition metal phosphides. For overall water splitting, the cell voltage is 1.65 V for Fe-CoP NFs at a current density of 10 mA cm<sup>−2</sup>, much superior to what is observed for the classical nanocubic structures. Fe-CoP NFs show no activity degradation up to 100 h which contrasts sharply with the rapidly decaying performance of noble metal catalyst reference. The superior electrocatalytic performance of Fe-CoP NFs due to abundant accessible active sites, reduced kinetic energy barrier, and preferable *O-containing intermediate adsorption is demonstrated through experimental observations and theoretical calculations. Our findings could provide a potential method for the preparation of multifunctional material with hollow structures and offer more hopeful prospects for obtaining efficient earth-abundant catalysts for water splitting.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12747","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141113773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Mo2B2O2 MBene for Efficient Electrochemical CO Reduction to C2 Chemicals: Computational Exploration","authors":"Bikun Zhang, Jianwen Jiang","doi":"10.1002/eem2.12738","DOIUrl":"10.1002/eem2.12738","url":null,"abstract":"<p>Emerging as a new class of two-dimensional materials with atomically thin layers, MBenes have great potential for many important applications such as energy storage and electrocatalysis. Toward mitigating carbon footprint, there has been increasing interest in CO<sub>2</sub>/CO conversion on MBenes, but mostly focused on C<sub>1</sub> products. C<sub>2+</sub> chemicals generally possess higher energy densities and wider applications than C<sub>1</sub> counterparts. However, C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process. Here, we explore electrochemical CO reduction reaction to C<sub>2</sub> chemicals on Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> MBene via density-functional theory calculations. Remarkably, the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process, making Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> an efficient catalyst for C–C coupling. Among C<sub>1</sub> and C<sub>2</sub> chemicals, ethanol is predicted to be the primary product. Furthermore, by charge and bond analysis, it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate *COH than other C<sub>1</sub> intermediates, which is responsible for the facile C–C coupling. From an atomic scale, this work provides microscopic insight into C–C coupling process and suggests Mo<sub>2</sub>B<sub>2</sub>O<sub>2</sub> a promising catalyst for electrochemical CO reduction to C<sub>2</sub> chemicals.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12738","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140969166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"High-Safety Anode Materials for Advanced Lithium-Ion Batteries","authors":"Kai Yuan, Yu Lin, Xiang Li, Yufeng Ding, Peng Yu, Jian Peng, Jiazhao Wang, HuaKun Liu, Shixue Dou","doi":"10.1002/eem2.12759","DOIUrl":"10.1002/eem2.12759","url":null,"abstract":"<p>Lithium-ion batteries (LIBs) play a pivotal role in today's society, with widespread applications in portable electronics, electric vehicles, and smart grids. Commercial LIBs predominantly utilize graphite anodes due to their high energy density and cost-effectiveness. Graphite anodes face challenges, however, in extreme safety-demanding situations, such as airplanes and passenger ships. The lithiation of graphite can potentially form lithium dendrites at low temperatures, causing short circuits. Additionally, the dissolution of the solid-electrolyte-interphase on graphite surfaces at high temperatures can lead to intense reactions with the electrolyte, initiating thermal runaway. This review introduces two promising high-safety anode materials, Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub>. Both materials exhibit low tendencies towards lithium dendrite formation and have high onset temperatures for reactions with the electrolyte, resulting in reduced heat generation and significantly lower probabilities of thermal runaway. Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub> offer enhanced safety characteristics compared to graphite, making them suitable for applications with stringent safety requirements. This review provides a comprehensive overview of Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> and TiNb<sub>2</sub>O<sub>7</sub>, focusing on their material properties and practical applicability. It aims to contribute to the understanding and development of high-safety anode materials for advanced LIBs, addressing the challenges and opportunities associated with their implementation in real-world applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12759","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140967192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Accelerating the Screening of Modified MA2Z4 Catalysts for Hydrogen Evolution Reaction by Deep Learning-Based Local Geometric Analysis","authors":"Jingnan Zheng, Shibin Wang, Shengwei Deng, Zihao Yao, Junhua Hu, Jianguo Wang","doi":"10.1002/eem2.12743","DOIUrl":"10.1002/eem2.12743","url":null,"abstract":"<p>Machine learning (ML) integrated with density functional theory (DFT) calculations have recently been used to accelerate the design and discovery of single-atom catalysts (SACs) by establishing deep structure–activity relationships. The traditional ML models are always difficult to identify the structural differences among the single-atom systems with different modification methods, leading to the limitation of the potential application range. Aiming to the structural properties of several typical two-dimensional MA<sub>2</sub>Z<sub>4</sub>-based single-atom systems (bare MA<sub>2</sub>Z<sub>4</sub> and metal single-atom doped/supported MA<sub>2</sub>Z<sub>4</sub>), an improved crystal graph convolutional neural network (CGCNN) classification model was employed, instead of the traditional machine learning regression model, to address the challenge of incompatibility in the studied systems. The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer, surface layer, and bulk layer (ASB-GCNN). Through ML and DFT calculations, five potential single-atom hydrogen evolution reaction (HER) catalysts were screened from chemical space of 600 MA<sub>2</sub>Z<sub>4</sub>-based materials, especially V<sub>1</sub>/HfSn<sub>2</sub>N<sub>4</sub>(S) with high stability and activity (Δ<i>G</i><sub><i>H</i>*</sub> is 0.06 eV). Further projected density of states (pDOS) analysis in combination with the wave function analysis of the SAC-H bond revealed that the SAC-<i>dz</i><sup>2</sup> orbital coincided with the H-<i>s</i> orbital around the energy level of −2.50 eV, and orbital analysis confirmed the formation of σ bonds. This study provides an efficient multistep screening design framework of metal single-atom catalyst for HER systems with similar two-dimensional supports but different geometric configurations.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12743","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140974087","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rui Li, Yulei Shi, Famin Yu, Rui Wang, Haitao Yan, Boon K. Teo, Zhigang Wang
{"title":"Understanding Bonding Nature of α-Keggin Polyoxometalates [XW12O40]n− (X = Al, Si, P, S): A Generalized Superatomic Perspective","authors":"Rui Li, Yulei Shi, Famin Yu, Rui Wang, Haitao Yan, Boon K. Teo, Zhigang Wang","doi":"10.1002/eem2.12754","DOIUrl":"10.1002/eem2.12754","url":null,"abstract":"<p>α-Keggin polyoxometalates (POMs) [XW<sub>12</sub>O<sub>40</sub>]<sup>n−</sup> (X = Al, Si, P, S) are widely used in batteries owing to their remarkable redox activity. However, the mechanism underlying the applications appears inconsistent with the widely accepted covalent bonding nature. Here, first-principles calculations show that XW<sub>12</sub> are core–shell structures composed of a shell and an XO<sub>4</sub><sup>n−</sup> core, both are stabilized by covalent interactions. Interestingly, owing to the presence of a substantial number of electrons in W<sub>12</sub>O<sub>36</sub> shell, the frontier molecular orbitals of XW<sub>12</sub> are not only strongly delocalized but also exhibit superatomic properties with high-angular momentum electrons that do not conform to the Jellium model. Detailed analysis indicates that energetically high lying filled molecular orbitals (MOs) have reached unusually high-angular momentum characterized by quantum number K or higher, allowing for the accommodation of numerous electrons. This attribute confers strong electron acceptor ability and redox activity to XW<sub>12</sub>. Moreover, electrons added to XW<sub>12</sub> still occupy the K orbitals and will not cause rearrangement of the MOs, thereby maintaining the stability of these structures. Our findings highlight the structure–activity relationship and provide a direction for tailor-made POMs with specific properties at atomic level.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12754","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140975788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Outstanding Lithium Storage Performance of a Copper-Coordinated Metal-Covalent Organic Framework as Anode Material for Lithium-Ion Batteries","authors":"Derong Luo, Huizi Zhao, Feng Liu, Hai Xu, Xiaoyu Dong, Bing Ding, Hui Dou, Xiaogang Zhang","doi":"10.1002/eem2.12732","DOIUrl":"10.1002/eem2.12732","url":null,"abstract":"<p>Metal-covalent organic frameworks (MCOF) as a bridge between covalent organic framework (COF) and metal organic framework (MOF) possess the characteristics of open metal sites, structure stability, crystallinity, tunability as well as porosity, but still in its infancy. In this work, a covalent organic framework DT-COF with a keto-enamine structure synthesized from the condensation of 3,3′-dihydroxybiphenyl diamine (DHBD) and triformylphloroglucinol (TFP) was coordinated with Cu<sup>2+</sup> by a simple post-modification method to a obtain a copper-coordinated metal-covalent organic framework of Cu-DT COF. The isomerization from a keto-enamine structure of DT-COF to a enol-imine structure of Cu-DT COF is induced due to the coordination interaction of Cu<sup>2+</sup>. The structure change of Cu-DT COF induces the change of the electron distribution in the Cu-DT COF, which greatly promotes the activation and deep Li-storage behavior of the COF skeleton. As anode material for lithium-ion batteries (LIBs), Cu-DT COF exhibits greatly improved electrochemical performance, retaining the specific capacities of 760 mAh g<sup>−1</sup> after 200 cycles and 505 mAh g<sup>−1</sup> after 500 cycles at a current density of 0.5 A g<sup>−1</sup>. The preliminary lithium storage mechanism studies indicate that Cu<sup>2+</sup> is also involved in the lithium storage process. A possible mechanism for Cu-DT COF was proposed on the basis of FT-IR, XPS, EPR characterization and electrochemical analysis. This work enlightens a novel strategy to improve the energy storage performance of COF and promotes the application of COF and MCOF in LIBs.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12732","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140974473","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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":"Hydrogen Spillover Effect in Electrocatalysis: Delving into the Mysteries of the Atomic Migration","authors":"Ashish Gaur, Jatin Sharma, HyukSu Han","doi":"10.1002/eem2.12761","DOIUrl":"10.1002/eem2.12761","url":null,"abstract":"<p>Hydrogen spillover effect has recently garnered a lot of attention in the field of electrocatalytic hydrogen evolution reactions. A new avenue for understanding the dynamic behavior of atomic migration in which hydrogen atoms moving on a catalyst surface was opened up by the setup of the word “hydrogen spillover.” However, there is currently a dearth of thorough knowledge regarding the hydrogen spillover effect. Currently, the advancement of sophisticated characterization procedures offers progressively useful information to enhance our grasp of the hydrogen spillover effect. The understanding of material fabrication for hydrogen spillover effect has erupted. Considering these factors, we made an effort to review most of the articles published on the hydrogen spillover effect and carefully analyzed the aspect of material fabrication. All of our attention has been directed toward the molecular pathway that leads to improve hydrogen evolution reactions performance. In addition, we have attempted to elucidate the spillover paths through the utilization of DFT calculations. Furthermore, we provide some preliminary research suggestions and highlight the opportunities and obstacles that are still to be confronted in this study area.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12761","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140972911","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shiyu Wei, Tuomas Haggren, Zhe Li, Hark Hoe Tan, Chennupati Jagadish, Antonio Tricoli, Lan Fu
{"title":"Ultrasensitive Indium Phosphide Nanomembrane Wearable Gas Sensors","authors":"Shiyu Wei, Tuomas Haggren, Zhe Li, Hark Hoe Tan, Chennupati Jagadish, Antonio Tricoli, Lan Fu","doi":"10.1002/eem2.12763","DOIUrl":"10.1002/eem2.12763","url":null,"abstract":"<p>Air quality is deteriorating due to continuing urbanization and industrialization. In particular, nitrogen dioxide (NO<sub>2</sub>) is a biologically and environmentally hazardous byproduct from fuel combustion that is ubiquitous in urban life. To address this issue, we report a high-performance flexible indium phosphide nanomembrane NO<sub>2</sub> sensor for real-time air quality monitoring. An ultralow limit of detection of ~200 ppt and a fast response have been achieved with this device by optimizing the film thickness and doping concentration during indium phosphide epitaxy. By varying the film thickness, a dynamic range of values for NO<sub>2</sub> detection from parts per trillion (ppt) to parts per million (ppm) level have also been demonstrated under low bias voltage and at room temperature without additional light activation. Flexibility measurements show an adequately stable response after repeated bending. On-site testing of the sensor in a residential kitchen shows that NO<sub>2</sub> concentration from the gas stove emission could exceed the NO<sub>2</sub> Time Weighted Average limit, i.e., 200 ppb, highlighting the significance of real-time monitoring. Critically, the indium phosphide nanomembrane sensor element cost is estimated at <0.1 US$ due to the miniatured size, nanoscale thickness, and ease of fabrication. With these superior performance characteristics, low cost, and real-world applicability, our indium phosphide nanomembrane sensors offer a promising solution for a variety of air quality monitoring applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12763","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140974683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pejman Salimi, Willem Vercruysse, Susana Chauque, Saeed Yari, Eleonora Venezia, Amine Lataf, Nahal Ghanemnia, Muhammad Shajih Zafar, Mohammadhosein Safari, An Hardy, Remo Proietti Zaccaria, Dries Vandamme
{"title":"Lithium-Metal-Free Sulfur Batteries with Biochar and Steam-Activated Biochar-Based Anodes from Spent Common Ivy","authors":"Pejman Salimi, Willem Vercruysse, Susana Chauque, Saeed Yari, Eleonora Venezia, Amine Lataf, Nahal Ghanemnia, Muhammad Shajih Zafar, Mohammadhosein Safari, An Hardy, Remo Proietti Zaccaria, Dries Vandamme","doi":"10.1002/eem2.12758","DOIUrl":"10.1002/eem2.12758","url":null,"abstract":"<p>Lithium-sulfur batteries are emerging as sustainable replacements for current lithium-ion batteries. The commercial viability of this novel type of battery is still under debate due to the extensive use of highly reactive lithium-metal anodes and the complex electrochemistry of the sulfur cathode. In this research, a novel sulfur-based battery has been proposed that eliminates the need for metallic lithium anodes and other critical raw materials like cobalt and graphite, replacing them with biomass-derived materials. This approach presents numerous benefits, encompassing ample availability, cost-effectiveness, safety, and environmental friendliness. In particular, two types of biochar-based anode electrodes (non-activated and activated biochar) derived from spent common ivy have been investigated as alternatives to metallic lithium. We compared their structural and electrochemical properties, both of which exhibited good compatibility with the typical electrolytes used in sulfur batteries. Surprisingly, while steam activation results in an increased specific surface area, the non-activated ivy biochar demonstrates better performance than the activated biochar, achieving a stable capacity of 400 mA h g<sup>−1</sup> at 0.1 A g<sup>−1</sup> and a long lifespan (>400 cycles at 0.5 A g<sup>−1</sup>). Our results demonstrate that the presence of heteroatoms, such as oxygen and nitrogen positively affects the capacity and cycling performance of the electrodes. This led to increased d-spacing in the graphitic layer, a strong interaction with the solid electrolyte interphase layer, and improved ion transportation. Finally, the non-activated biochar was successfully coupled with a sulfur cathode to fabricate lithium-metal-free sulfur batteries, delivering a specific energy density of ~600 Wh kg<sup>−1</sup>.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12758","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140972028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}