Juan Meng, Huidong Liu, Jianing Xu, Yu-Jiao Lou, Haixin Sun, Bo Jiang, Yongzhuang Liu, Hengfei Qin, Shuo Dou, Haipeng Yu
{"title":"Nanocarbon catalysts with co‐active S−P−C sites enhance metal‐free direct oxidation of alcohols","authors":"Juan Meng, Huidong Liu, Jianing Xu, Yu-Jiao Lou, Haixin Sun, Bo Jiang, Yongzhuang Liu, Hengfei Qin, Shuo Dou, Haipeng Yu","doi":"10.1002/sus2.221","DOIUrl":"https://doi.org/10.1002/sus2.221","url":null,"abstract":"In this study, a sulfur–phosphorus co‐doped nanocarbon (SPC) catalyst was synthesized using a straightforward one‐step colloidal carbonization method and demonstrated high performance in the metal‐free direct oxidation of alcohols to aldehydes. This metal‐free SPC catalyst showed exceptional efficiency, achieving a conversion rate of 90% for benzyl alcohol and a selectivity of 94% toward benzaldehyde within only 1 h at 130°C. Moreover, it displays exceptional cycle stability and a high turnover frequency (17.1 × 10−3 mol g−1 h−1). Theoretical analysis suggested that the catalyst's superior performance is attributed to the presence of unsaturated edge defects and S−P− moieties, which increase the density of states at the Fermi level, lower the band gap energy, and promote electron localization. Additionally, the doping introduces cooperative co‐active S−P−C sites, facilitating a synergistic multisite catalytic effect that lowers the energy barriers. These findings represent a significant advancement in the field of metal‐free direct alcohol oxidation.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"31 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141645679","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Flexible mica films coated by magnetron sputtered insulating layers for high‐temperature capacitive energy storage","authors":"Chao Yin, Tiandong Zhang, Changhai Zhang, Yue Zhang, Chang Kyu Jeong, Geon‐Tae Hwang, Q. Chi","doi":"10.1002/sus2.228","DOIUrl":"https://doi.org/10.1002/sus2.228","url":null,"abstract":"High‐temperature energy storage performance of dielectric capacitors is crucial for the next generation of power electronic devices. However, conduction losses rise sharply at elevated temperature, limiting the application of energy storage capacitors. Here, the mica films magnetron sputtered by different insulating layers are specifically investigated, which exhibit the excellent high‐temperature energy storage performance. The experimental results revealed that the PbZrO3/Al2O3/PbZrO3 (PZO/AO/PZO) interface insulating layers can effectively reduce the high‐temperature leakage current and conduction loss of the composite films. Consequently, the ultrahigh energy storage density (Wrec) and charge‒discharge efficiency (η) can be achieved simultaneously in the flexible mica‐based composite films. Especially, PZO/AO/PZO/mica/PZO/AO/PZO (PAPMPAP) films possess excellent Wrec of 27.5 J/cm3 and η of 87.8% at 200°C, which are significantly better than currently reported high‐temperature capacitive energy storage dielectric materials. Together with outstanding power density and electrical cycling stability, the flexible films in this work have great application potential in high‐temperature energy storage capacitors. Moreover, the magnetron sputtering technology can deposit large‐area nanoscale insulating layers on the surface of capacitor films, which can provide technical support for the industrial production of capacitors.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"45 4","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141655545","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Taehee An, Chengkai Xia, Minyeong Je, Hyunjung Lee, Seulgi Ji, Min‐Cheol Kim, S. Surendran, Mi-Kyung Han, Jaehyoung Lim, Dong‐Kyu Lee, Joonyoung Kim, Tae-Hoon Kim, Heechae Choi, Jung Kyu Kim, U. Sim
{"title":"V2O3/VN electrocatalysts with coherent heterogeneous interfaces for selecting low‐energy nitrogen reduction pathways","authors":"Taehee An, Chengkai Xia, Minyeong Je, Hyunjung Lee, Seulgi Ji, Min‐Cheol Kim, S. Surendran, Mi-Kyung Han, Jaehyoung Lim, Dong‐Kyu Lee, Joonyoung Kim, Tae-Hoon Kim, Heechae Choi, Jung Kyu Kim, U. Sim","doi":"10.1002/sus2.226","DOIUrl":"https://doi.org/10.1002/sus2.226","url":null,"abstract":"Electrochemical nitrogen reduction reaction (NRR) is a sustainable alternative to the Haber‒Bosch process for ammonia (NH3) production. However, the significant uphill energy in the multistep NRR pathway is a bottleneck for favorable serial reactions. To overcome this challenge, we designed a vanadium oxide/nitride (V2O3/VN) hybrid electrocatalyst in which V2O3 and VN coexist coherently at the heterogeneous interface. Since single‐phase V2O3 and VN exhibit different surface catalytic kinetics for NRR, the V2O3/VN hybrid electrocatalyst can provide alternating reaction pathways, selecting a lower energy pathway for each material in the serial NRR pathway. As a result, the ammonia yield of the V2O3/VN hybrid electrocatalyst was 219.6 µg h−1 cm−2, and the Faradaic efficiency was 18.9%, which is much higher than that of single‐phase VN, V2O3, and VNxOy solid solution catalysts without heterointerfaces. Density functional theory calculations confirmed that the composition of these hybrid electrocatalysts allows NRR to proceed from a multistep reduction reaction to a low‐energy reaction pathway through the migration and adsorption of intermediate species. Therefore, the design of metal oxide/nitride hybrids with coherent heterointerfaces provides a novel strategy for synthesizing highly efficient electrochemical catalysts that induce steps favorable for the efficient low‐energy progression of NRR.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"118 18","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141656788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Breaking barriers: Sunlight‐activated self‐healing polymers with unprecedented photoaging resistance","authors":"Yan Mei Li, Z. Zhang, M. Rong, Ming Qiu Zhang","doi":"10.1002/sus2.227","DOIUrl":"https://doi.org/10.1002/sus2.227","url":null,"abstract":"Sunlight‐triggered self‐healing of polymers has attractive advantages, but the same illumination inevitably causes photoaging. The resulting properties deterioration and shortened lifespan run counter to the desire for self‐healing. Herein, the authors propose an innovative solution by introducing carbazolyl‐based dithiocarbamate units. The proof‐of‐concept crosslinked poly(carbazolyl dithiocarbamates‐urethane) shows that the multitasking reactivities of the dynamic bonds stimulated by the sun's ultraviolet rays concurrently implement self‐healing and improve the photoaging resistance. As reflected by the xenon weatherometer measurements, it retains 73.5% of the original strength after 576 h owing to the effects of hydroperoxide intermediates elimination and fluorescence emission. The anti‐photoaging ability is far superior to the control filled with commercial stabilizer. Meantime, networks rearrangement via dynamic exchange reactions among the sunlight‐sensitive dithiocarbamates and long‐range free radicals transfer are allowed in surface layer and the interior, so that the cracks up to 8.5 mm deep are repaired. The work provides a feasible way to break the bottleneck in application of photochemical self‐healing polymers.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"81 7","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141657951","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tianyi Wang, Yimeng Zhang, Xueyan Huang, Peifeng Su, M. Xiao, Shuanjin Wang, Sheng Huang, Dongmei Han, Yuezhong Meng
{"title":"Designing weakly and strongly solvating polymer electrolytes: Systematically boosting high‐voltage lithium metal batteries","authors":"Tianyi Wang, Yimeng Zhang, Xueyan Huang, Peifeng Su, M. Xiao, Shuanjin Wang, Sheng Huang, Dongmei Han, Yuezhong Meng","doi":"10.1002/sus2.219","DOIUrl":"https://doi.org/10.1002/sus2.219","url":null,"abstract":"Practical high‐voltage lithium metal batteries hold promise for high energy density applications, but face stability challenges in electrolytes for both 4 V‐class cathodes and lithium anode. To address this, we delve into the positive impacts of two crucial moieties in electrolyte chemistry: fluorine atom (‐F) and cyano group (‐CN) on the electrochemical performance of polyether electrolytes and lithium metal batteries. Cyano‐bearing polyether electrolytes possess strong solvation, accelerating Li+ desolvation with minimal SEI impact. Fluorinated polyether electrolytes possess weak solvation, and stabilize the lithium anode via preferential decomposition of F‐segment, exhibiting nearly 6000‐h stable cycling of lithium symmetric cell. Furthermore, the electron‐withdrawing properties of ‐F and ‐CN groups significantly bolster the high‐voltage tolerance of copolymer electrolyte, extending its operational range up to 5 V. This advancement enables the development of 4 V‐class lithium metal batteries compatible with various cathodes, including 4.45 V LiCoO2, 4.5 V LiNi0.8Co0.1Mn0.1O2, and 4.2 V LiNi0.5Co0.2Mn0.3O2. These findings provide insights into design principles centered around polymer components for high‐performance polymer electrolytes.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"11 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141658812","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuetong Zhou, Ding Zhang, Shuai Zhang, Yuqing Liu, Rujun Ma, Gordon Wallace, Jun Chen
{"title":"Highly stretchable double‐network gel electrolytes integrated with textile electrodes for wearable thermo‐electrochemical cells","authors":"Yuetong Zhou, Ding Zhang, Shuai Zhang, Yuqing Liu, Rujun Ma, Gordon Wallace, Jun Chen","doi":"10.1002/sus2.225","DOIUrl":"https://doi.org/10.1002/sus2.225","url":null,"abstract":"Thermo‐electrochemical cells (TECs) provide a new potential for self‐powered devices by converting heat energy into electricity. However, challenges still remain in the fabrication of flexible and tough gel electrolytes and their compatibility with redox actives; otherwise, contact problems exist between electrolytes and electrodes during stretching or twisting. Here, a novel robust and neutral hydrogel with outstanding stretchability was developed via double‐network of crosslinked carboxymethyl chitosan and polyacrylamide, which accommodated both n‐type (Fe2+/Fe3+) and p‐type ([Fe(CN)6]3−/[Fe(CN)6]4−) redox couples and maintained stretchability (>300%) and recoverability (95% compression). Moreover, poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) textile electrodes with porous structure are integrated into gel electrolytes that avoid contact issues and effectively boost the Pmax of n‐ and p‐type thermocell by 76% and 26%, respectively. The optimized thermocell exhibits a quick current density response and is continually fully operational under deformations, which satisfies the working conditions of wearable devices. Multiple thermocells (four pairs) are effectively connected in alternating single n‐ and p‐type cells in series and outputted nearly 74.3 mV at ΔT = 10°C. The wearable device is manufactured into a soft‐pack thermocells to successfully harvest human body heat and illuminate an LED, demonstrating the potential of the actual application of the thermocell devices.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"2 18","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141662079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Air‐stable Li3.12P0.94Bi0.06S3.91I0.18 solid‐state electrolyte with high ionic conductivity and lithium anode compatibility toward high‐performance all‐solid‐state lithium metal batteries","authors":"Daokuan Jin, Haodong Shi, Yuxin Ma, Yangyang Liu, Yang Wang, Yanfeng Dong, Mingbo Wu, Zhong‐Shuai Wu","doi":"10.1002/sus2.218","DOIUrl":"https://doi.org/10.1002/sus2.218","url":null,"abstract":"Sulfide solid‐state electrolytes (SSEs) with superior ionic conductivity and processability are highly promising candidates for constructing all‐solid‐state lithium metal batteries (ASSLMBs). However, their practical applications are limited by their intrinsic air instability and serious interfacial incompatibility. Herein, a novel glass‐ceramic electrolyte Li3.12P0.94Bi0.06S3.91I0.18 was synthesized by co‐doping Li3PS4 with Bi and I for high‐performance ASSLMBs. Owing to the strong Bi‒S bonds that are thermodynamically stable to water, increased unit cell volume and Li+ concentration caused by P5+ substitution with Bi3+, and the in situ formed robust solid electrolyte interphase layer LiI at lithium surface, the as‐prepared Li3.12P0.94Bi0.06S3.91I0.18 SSE achieved excellent air stability with a H2S concentration of only 0.205 cm3 g−1 (after 300 min of air exposure), outperforming Li3PS4 (0.632 cm3 g−1) and the most reported sulfide SSEs, together with high ionic conductivity of 4.05 mS cm−1. Furthermore, the Li3.12P0.94Bi0.06S3.91I0.18 effectively improved lithium metal stability. With this SSE, an ultralong cyclability of 700 h at 0.1 mA cm−2 was realized in a lithium symmetrical cell. Moreover, the Li3.12P0.94Bi0.06S3.91I0.18‐based ASSLMBs with LiNi0.8Mn0.1Co0.1O2 cathode achieved ultrastable capacity retention rate of 95.8% after 300 cycles at 0.1 C. This work provides reliable strategy for designing advanced sulfide SSEs for commercial applications in ASSLMBs.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"3 17","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141667985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qianru Rao, Yujie Xu, Xiaorong Wang, Hang Luo, Haoqi Li, Jingyuan Xiong, Huile Gao, G. Cheng
{"title":"Construction of an intranasal drug delivery system with hypothalamus‐targeting nanoparticles","authors":"Qianru Rao, Yujie Xu, Xiaorong Wang, Hang Luo, Haoqi Li, Jingyuan Xiong, Huile Gao, G. Cheng","doi":"10.1002/sus2.222","DOIUrl":"https://doi.org/10.1002/sus2.222","url":null,"abstract":"Dysfunction of the hypothalamus is associated with endocrine imbalances, growth abnormalities, and reproductive disorders. However, there is a lack of targeted treatment strategies focused on the hypothalamus. In this study, we constructed a multifunctional nanocarrier system (S@ANP) to directly target the hypothalamic neurokinin receptor 3 (NK3R) via an intranasal delivery strategy. This system could overcome the primary obstacles in drug delivery for hypothalamus‐related diseases. Under the guidance of a modified (Trp7, β‐Ala8)‐neurokinin A (4‐10) peptide with cysteine, nanoparticles encapsulated with SB222200, an NK3R inhibitor, were found to readily penetrate hypothalamic cells with substantial loading capacity, encapsulation efficiency, and sustained release in vitro. Moreover, intranasal delivery represents an optimal delivery strategy that allows for a significant reduction in oral dosage and enables nanoparticles to bypass the blood‒brain barrier and target relevant parts of the brain. The mucolytic agent N‐acetyl‐L‐cysteine (NAC) was loaded into the nanoparticles (S@ANP + NAC) to increase mucosal solubility and intranasal delivery efficiency. In vivo evaluations showed that S@ANP + NAC could effectively target the hypothalamus and modulate NK3R‐regulated hypothalamic functions in mice. Due to its high hypothalamic targeting efficiency and low toxicity, this intranasal nanoparticle drug delivery system may serve as a potential strategy for precision therapy of hypothalamic disorders.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"66 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141687014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuan-You Peng, Yi-Han Fu, Meimei Yu, Lei Zhao, Huanzhong Zeng, Shengtao Niu, Jie Zhang, Junlong Chen, Guang Liu, Youzhi Wu, F. Ran
{"title":"High micropore‐utilization carbon aerogel with controlled nanostructures via adjusting aggregation state of polyacrylonitrile for energy storage systems","authors":"Yuan-You Peng, Yi-Han Fu, Meimei Yu, Lei Zhao, Huanzhong Zeng, Shengtao Niu, Jie Zhang, Junlong Chen, Guang Liu, Youzhi Wu, F. Ran","doi":"10.1002/sus2.217","DOIUrl":"https://doi.org/10.1002/sus2.217","url":null,"abstract":"Designing and optimizing the pore structure of porous carbon electrodes is essential for diverse energy storage systems. In this study, an innovative approach spray phase‐inversion strategy was developed for the rapid and efficient fabrication of controlled porous carbon aerogel. Moreover, the aggregation structure of polyacrylonitrile is controlled by adjusting the Hansen's solubility parameter, thereby regulating the electrode material structure. Furthermore, the theoretical analysis of the spray phase‐inversion process revealed that this regulation process is jointly regulated by solvent hydrodynamic diameter and phase‐inversion kinetics. Through optimization, a novel porous carbon material was obtained that exhibited excellent performance as an electrode material. When utilized in supercapacitors for energy storage, it demonstrated a high specific capacitance of 373.1 F g−1 in a 6 M KOH electrolyte solution. Simultaneously, it has been observed that the preparation strategy for porous electrodes offers notable advantages in terms of excellent designability, broad universality, simplicity, and high efficiency, thereby holding promise for large‐scale fabrication of diverse porous electrode materials and various types of electrodes for diverse energy storage applications.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":"47 37","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141339503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"New paradigms of water‐enabled electrical energy generation","authors":"Zhengtong Li, Tao Yang, Jia‐Han Zhang, Taotao Meng, Saad Melhi, Jungmok You, Miharu Eguchi, Likun Pan, Yusuke Yamauchi, Xingtao Xu","doi":"10.1002/sus2.206","DOIUrl":"https://doi.org/10.1002/sus2.206","url":null,"abstract":"Nanotechnology‐inspired small‐sized water‐enabled electricity generation (WEG) has sparked widespread research interest, especially when applied as an electricity source for off‐grid low‐power electronic equipment and systems. Currently, WEG encompasses a wide range of physical phenomena, generator structures, and power generation environments. However, a systematic framework to clearly describe the connections and differences between these technologies is unavailable. In this review, a comprehensive overview of generator technologies and the typical mechanisms for harvesting water energy is provided. Considering the different roles of water in WEG processes, the related technologies are presented as two different scenarios. Moreover, a detailed analysis of the electrical potential formation in each WEG process is presented, and their similarities and differences are elucidated. Furthermore, a comprehensive compilation of advanced generator architectures and system designs based on hydrological cycle processes is presented, along with their respective energy efficiencies. These nanotechnology‐inspired small‐sized WEG devices show considerable potential for applications in the Internet of Things ecosystem (i.e., microelectronic devices, integrated circuits, and smart clothing). Finally, the prospects and future challenges of WEG devices are also summarized.","PeriodicalId":506315,"journal":{"name":"SusMat","volume":" 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141365230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}