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Deciphering orbital hybridization in heterogeneous catalysis 破译异相催化中的轨道杂化
Electron Pub Date : 2024-01-24 DOI: 10.1002/elt2.16
Xiaoyang Yue, Lei Cheng, Eszter Baráth, Rajenahally V. Jagadeesh, Quanjun Xiang
{"title":"Deciphering orbital hybridization in heterogeneous catalysis","authors":"Xiaoyang Yue,&nbsp;Lei Cheng,&nbsp;Eszter Baráth,&nbsp;Rajenahally V. Jagadeesh,&nbsp;Quanjun Xiang","doi":"10.1002/elt2.16","DOIUrl":"10.1002/elt2.16","url":null,"abstract":"<p>The catalytic coordinate is essentially the evolving frontier orbital interaction while feeding with catalytic materials and adsorbates under proper reaction conditions. The heterogeneous catalytic reaction mechanism involves the initial adsorption and activation of reactants, subsequent intermediate transformation, final target product desorption, and regeneration of catalytic materials. In these catalytic processes, interaction modulations in terms of orbital hybridization/coupling allow an intrinsic control on both thermodynamics and kinetics. Concerned charge transfer and redistribution, orbital splitting and rearrangement with specific orientation, and spin change and crossover pose a formidable challenge on mechanism elucidation; it is hard to precisely correlate the apparent activity and selectivity, let alone rational modulations on it. Therefore, deciphering the orbital couplings inside a catalytic round is highly desirable and the dependent descriptor further provides in-depth insights into catalyst design at the molecule orbital level. This review hopes to provide a comprehensive understanding on orbital hybridizations, modulations, and correlated descriptors in heterogeneous catalysis.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.16","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139601171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Improving sulfur transformation of lean electrolyte lithium–sulfur battery using nickel nanoparticles encapsulated in N-doped carbon nanotubes 使用包裹在掺 N 碳纳米管中的纳米镍颗粒改善贫电解质锂硫电池的硫转化性能
Electron Pub Date : 2024-01-18 DOI: 10.1002/elt2.19
Ze Zhang, Yuqing Xu, Donggen Xiong, Ji Yu, Jianxin Cai, Yizhong Huang, Zhenyu Yang
{"title":"Improving sulfur transformation of lean electrolyte lithium–sulfur battery using nickel nanoparticles encapsulated in N-doped carbon nanotubes","authors":"Ze Zhang,&nbsp;Yuqing Xu,&nbsp;Donggen Xiong,&nbsp;Ji Yu,&nbsp;Jianxin Cai,&nbsp;Yizhong Huang,&nbsp;Zhenyu Yang","doi":"10.1002/elt2.19","DOIUrl":"10.1002/elt2.19","url":null,"abstract":"<p>Efficient redox reactions of lean electrolyte lithium–sulfur (Li–S) batteries highly rely on rational catalyst design. Herein, we report an electrocatalyst based on N-doped carbon nanotubes (CNT)-encapsulated Ni nanoparticles (Ni@NCNT) as kinetics regulators for Li–S batteries to propel the polysulfide-involving multiphase transformation. Moreover, such a CNT-encapsulation strategy greatly prevents the aggregation of Ni nanoparticles and enables the extraordinary structural stability of the hybrid electrocatalyst, which guarantees its persistent catalytic activity on sulfur redox reactions. When used as a modified layer on a commercial separator, the Ni@NCNT interlayer contributes to stabilizing S cathode and Li anode by significantly retarding the shuttle effect. The corresponding batteries with a 3.5 mg cm<sup>−2</sup> sulfur loading achieve the promising cycle stability with ∼85% capacity retention at the electrolyte/sulfur ratios of 5 and 3 μL mg<sup>−1</sup>. Even at a high loading of 12.2 mg cm<sup>−2</sup>, the battery affords an areal capacity of 7.5 mA h cm<sup>−2</sup>.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.19","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139616461","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unveiling the correlation between structural alterations and enhanced high-voltage cyclability in Na-deficient P3-type layered cathode materials via Li incorporation 通过掺入锂揭示缺钠 P3 型层状阴极材料的结构变化与增强高压循环性之间的相关性
Electron Pub Date : 2024-01-12 DOI: 10.1002/elt2.18
Xiaoxia Yang, Suning Wang, Hang Li, Jochi Tseng, Zhonghua Wu, Sylvio Indris, Helmut Ehrenberg, Xiaodong Guo, Weibo Hua
{"title":"Unveiling the correlation between structural alterations and enhanced high-voltage cyclability in Na-deficient P3-type layered cathode materials via Li incorporation","authors":"Xiaoxia Yang,&nbsp;Suning Wang,&nbsp;Hang Li,&nbsp;Jochi Tseng,&nbsp;Zhonghua Wu,&nbsp;Sylvio Indris,&nbsp;Helmut Ehrenberg,&nbsp;Xiaodong Guo,&nbsp;Weibo Hua","doi":"10.1002/elt2.18","DOIUrl":"10.1002/elt2.18","url":null,"abstract":"<p>With exceptional capacity during high-voltage cycling, P3-type Na-deficient layered oxide cathodes have captured substantial attention. Nevertheless, they are plagued by severe capacity degradation over cycling. In this study, tuning and optimizing the phase composition in layered oxides through Li incorporation are proposed to enhance the high-voltage stability. The structural dependence of layered Na<sub>2/3</sub>Li<sub><i>x</i></sub>Ni<sub>0.25</sub>Mn<sub>0.75</sub>O<sub>2+<i>δ</i></sub> oxides on the lithium content (0.0 ≤ <i>x</i> ≤ 1.0) offered during synthesis is investigated systematically on an atomic scale. Surprisingly, increasing the Li content triggers the formation of mixed P2/O3-type or P3/P2/O3-type layered phases. As the voltage window is 1.5–4.5 V, P3-type Na<sub>2/3</sub>Ni<sub>0.25</sub>Mn<sub>0.75</sub>O<sub>2</sub> (NL<sub>0.0</sub>NMO, <i>R</i><math>\u0000 <semantics>\u0000 <mrow>\u0000 <mover>\u0000 <mn>3</mn>\u0000 <mo>‾</mo>\u0000 </mover>\u0000 </mrow>\u0000 <annotation> $overline{3}$</annotation>\u0000 </semantics></math><i>m</i>) material exhibits a sequence of phase transformations throughout the process of (de)sodiation, that is, O3⇌P3⇌O3′⇌O3″. Such complicated phase transitions can be effectively suppressed in the Na<sub>2/3</sub>Li<sub>0.7</sub>Ni<sub>0.25</sub>Mn<sub>0.75</sub>O<sub>2.4</sub> (NL<sub>0.7</sub>NMO) oxide with P2/P3/O3-type mixed phases. Consequently, cathodes made of NL<sub>0.7</sub>NMO exhibit a substantially enhanced cyclic performance at high voltages compared to that of the P3-type layered NL<sub>0.0</sub>NMO cathode. Specifically, NL<sub>0.7</sub>NMO demonstrates an outstanding capacity retention of 98% after 10 cycles at 1 C within 1.5–4.5 V, much higher than that of NL<sub>0.0</sub>NMO (83%). This work delves into the intricate realm of bolstering the high-voltage durability of layered oxide cathodes, paving the way for advanced sodium-ion battery technologies.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.18","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139531791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Progress in MXene-based catalysts for oxygen evolution reaction 基于 MXene 的氧进化反应催化剂的研究进展
Electron Pub Date : 2023-12-30 DOI: 10.1002/elt2.17
Jieli Chen, Xiaohong Gao, Jing Li, Zhenye Kang, Juan Bai, Tianjiao Wang, Yuliang Yuan, Chenghang You, Yu Chen, Bao Yu Xia, Xinlong Tian
{"title":"Progress in MXene-based catalysts for oxygen evolution reaction","authors":"Jieli Chen,&nbsp;Xiaohong Gao,&nbsp;Jing Li,&nbsp;Zhenye Kang,&nbsp;Juan Bai,&nbsp;Tianjiao Wang,&nbsp;Yuliang Yuan,&nbsp;Chenghang You,&nbsp;Yu Chen,&nbsp;Bao Yu Xia,&nbsp;Xinlong Tian","doi":"10.1002/elt2.17","DOIUrl":"https://doi.org/10.1002/elt2.17","url":null,"abstract":"<p>Electrochemical water splitting for hydrogen generation is considered one of the most promising strategies for reducing the use of fossil fuels and storing renewable electricity in hydrogen fuel. However, the anodic oxygen evolution process remains a bottleneck due to the remarkably high overpotential of about 300 mV to achieve a current density of 10 mA cm<sup>−2</sup>. The key to solving this dilemma is the development of highly efficient catalysts with minimized overpotential, long-term stability, and low cost. As a new 2D material, MXene has emerged as an intriguing material for future energy conversion technology due to its benefits, including superior conductivity, excellent hydrophilic properties, high surface area, versatile chemical composition, and ease of processing, which make it a potential constituent of the oxygen evolution catalyst layer. This review aims to summarize and discuss the recent development of oxygen evolution catalysts using MXene as a component, emphasizing the synthesis and synergistic effect of MXene-based composite catalysts. Based on the discussions summarized in this review, we also provide future research directions regarding electronic interaction, stability, and structural evolution of MXene-based oxygen evolution catalysts. We believe that a broader and deeper research in this area could accelerate the discovery of efficient catalysts for electrochemical oxygen evolution.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.17","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139993970","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A common polar dye additive as corrosion inhibitor and leveling agent for stable aqueous zinc-ion batteries 一种常见的极性染料添加剂,可用作稳定的锌离子水电池的缓蚀剂和匀染剂
Electron Pub Date : 2023-12-26 DOI: 10.1002/elt2.21
Hao Wang, Chao Hu, Zefang Yang, Tingqing Wu, Yihu Li, Qi Zhang, Yougen Tang, Haiyan Wang
{"title":"A common polar dye additive as corrosion inhibitor and leveling agent for stable aqueous zinc-ion batteries","authors":"Hao Wang,&nbsp;Chao Hu,&nbsp;Zefang Yang,&nbsp;Tingqing Wu,&nbsp;Yihu Li,&nbsp;Qi Zhang,&nbsp;Yougen Tang,&nbsp;Haiyan Wang","doi":"10.1002/elt2.21","DOIUrl":"https://doi.org/10.1002/elt2.21","url":null,"abstract":"<p>The industrial application of zinc-ion batteries is restricted by irrepressible dendrite growth and side reactions that resulted from the surface heterogeneity of the commercial zinc electrode and the thermodynamic spontaneous corrosion in a weakly acidic aqueous electrolyte. Herein, a common polar dye, Procion Red MX-5b, with high polarity and asymmetric charge distribution is introduced into the zinc sulfate electrolyte, which can not only reconstruct the solvation configuration of Zn<sup>2+</sup> and strengthen hydrogen bonding to reduce the reactivity of free H<sub>2</sub>O but also homogenize interfacial electric field by its preferentially absorption on the zinc surface. The symmetric cell can cycle with a lower voltage hysteresis (78.4 mV) for 1120 times at 5 mA cm<sup>−2</sup> and Zn//NaV<sub>3</sub>O<sub>8</sub>·1.5H<sub>2</sub>O full cell can be cycled over 1000 times with high capacity (average 170 mAh g<sup>−1</sup>) at 4 A g<sup>−1</sup> in the compound electrolyte. This study provides a new perspective for additive engineering strategies of aqueous zinc-ion batteries.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.21","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139993873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An examination and prospect of stabilizing Li metal anode in lithium–sulfur batteries: A review of latest progress 锂硫电池中稳定锂金属阳极的研究与展望:最新进展综述
Electron Pub Date : 2023-11-28 DOI: 10.1002/elt2.13
Bingyan Song, Laisuo Su, Xi Liu, Wanjie Gao, Tao Wang, Yuan Ma, Yiren Zhong, Xin-Bing Cheng, Zhi Zhu, Jiarui He, Yuping Wu
{"title":"An examination and prospect of stabilizing Li metal anode in lithium–sulfur batteries: A review of latest progress","authors":"Bingyan Song,&nbsp;Laisuo Su,&nbsp;Xi Liu,&nbsp;Wanjie Gao,&nbsp;Tao Wang,&nbsp;Yuan Ma,&nbsp;Yiren Zhong,&nbsp;Xin-Bing Cheng,&nbsp;Zhi Zhu,&nbsp;Jiarui He,&nbsp;Yuping Wu","doi":"10.1002/elt2.13","DOIUrl":"https://doi.org/10.1002/elt2.13","url":null,"abstract":"<p>The Li metal anode emerges as a formidable competitor among anode materials for lithium–sulfur (Li-S) batteries; nevertheless, safety issues pose a significant hurdle in its path toward commercial viability. This review enumerates three historical challenges inherent to the Li metal anode: unavoidable volume expansion, multifunctional solid electrolyte interface formation, and uncontrollable lithium dendrite growth. In particular, when paired with a sulfur cathode, the Li anode presents an additional unique hurdle: the shuttle effect. To address these issues, this article offers a thorough examination of the latest innovations aimed at stabilizing the Li metal anode within Li-S batteries. We categorize these approaches into five classifications: liquid electrolyte optimization, enhancement of non-liquid-state electrolytes, Li metal surface modification, Li anode architecture design, and Li alloy improvement. For several noteworthy results within these categories, we have compiled their electrochemical performance into tables, facilitating direct comparison. This detailed analysis illuminates feasible strategies and suggests directions warranting further exploration for optimizing the capability and safety of Li metal anodes in Li-S batteries.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.13","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138454707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Back Cover Image, Volume 1, Number 2, November 2023 封底图片,第一卷,第2期,2023年11月
Electron Pub Date : 2023-11-28 DOI: 10.1002/elt2.24
Bingyan Song, Laisuo Su, Xi Liu, Wanjie Gao, Tao Wang, Yuan Ma, Yiren Zhong, Xin-Bing Cheng, Zhi Zhu, Jiarui He, Yuping Wu
{"title":"Back Cover Image, Volume 1, Number 2, November 2023","authors":"Bingyan Song,&nbsp;Laisuo Su,&nbsp;Xi Liu,&nbsp;Wanjie Gao,&nbsp;Tao Wang,&nbsp;Yuan Ma,&nbsp;Yiren Zhong,&nbsp;Xin-Bing Cheng,&nbsp;Zhi Zhu,&nbsp;Jiarui He,&nbsp;Yuping Wu","doi":"10.1002/elt2.24","DOIUrl":"https://doi.org/10.1002/elt2.24","url":null,"abstract":"<p>This picture mainly depicts the model of a Li-S battery circled by a Li metal ring, emphasizing the theme of Li metal anode in Li-S batteries. Some lithium dendrites are growing on the left of the ring while polysulfides composed of yellow balls(Sulfur ions) and metallic blue balls (lithium ions) are scattering on the right, precisely representing the lithium dendrites growing problem of Li metal anode and the shuttle effect as the unique problem in Li-S batteries. Meanwhile, the blue current on the ring implies the battery's operating status, echoing the journal's name,“<i>Electron</i>”.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.24","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138454711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cover Image, Volume 1, Number 2, November 2023 封面图片,第一卷,第2期,2023年11月
Electron Pub Date : 2023-11-28 DOI: 10.1002/elt2.23
Li Sun, Yating Li, Jiacheng Xie, Liqi Zhou, Peng Wang, Jian-Bin Xu, Yi Shi, Xinran Wang, Daowei He
{"title":"Cover Image, Volume 1, Number 2, November 2023","authors":"Li Sun,&nbsp;Yating Li,&nbsp;Jiacheng Xie,&nbsp;Liqi Zhou,&nbsp;Peng Wang,&nbsp;Jian-Bin Xu,&nbsp;Yi Shi,&nbsp;Xinran Wang,&nbsp;Daowei He","doi":"10.1002/elt2.23","DOIUrl":"https://doi.org/10.1002/elt2.23","url":null,"abstract":"<p>The cover image is the structure diagram of bottom-gate staggered OTFT with the circuit diagram as the background, where the channel material is a typical small-molecule C<sub>10</sub>-DNTT. The metal atoms can penetrate into the charge transport layer, with damage-free, via modulating organic crystal thickness during thermal evaporation of electrode. This could effectively reduce the contact resistance to aid the development of high-performance organic devices and circuits.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.23","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138454708","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dual surface/bulk engineering of Nb2O5 for high-rate sodium storage 高速储钠用Nb2O5双表面/体工程
Electron Pub Date : 2023-11-23 DOI: 10.1002/elt2.15
Yingjun Jiang, Xianluo Hu
{"title":"Dual surface/bulk engineering of Nb2O5 for high-rate sodium storage","authors":"Yingjun Jiang,&nbsp;Xianluo Hu","doi":"10.1002/elt2.15","DOIUrl":"https://doi.org/10.1002/elt2.15","url":null,"abstract":"<p>Orthorhombic Nb<sub>2</sub>O<sub>5</sub> is a highly promising fast-charging anode material for sodium-ion capacitors. However, its poor intrinsic electronic/ionic conductivity limits its performance. Here, we developed a one-step heat treatment method to create an N-doped carbon coating on the outside and S-doped Nb<sub>2</sub>O<sub>5</sub> on the inside (CN-SCN). Ionic liquids are used as the source of C/N/S, which synergistically enhance the surface and bulk electronic/ionic conductivity. The N-doped carbon coating on the surface exhibits excellent electronic conductivity and a low ion-diffusion barrier, thanks to the high nitrogen ratio and extremely low content (&lt;2 wt%). Auger electron spectroscopy analysis confirms that S atoms detach from the carbon chain of the ionic liquids and enter the bulk Nb<sub>2</sub>O<sub>5</sub>, resulting in S-doped Nb<sub>2</sub>O<sub>5</sub>, significantly facilitating reaction kinetics. The CN-SCN electrodes exhibit outstanding rate capability, achieving a capacity of up to 94 mAh g<sup>−1</sup> even at a high current rate of 50 C. When paired with activated carbon as the positive electrode, the sodium-ion capacitor with the CN-SCN anode exhibits a high-energy density of up to 59 Wh kg<sup>−1</sup> and a long cycle life with 73% capacity retention after 10,000 cycles. This work opens up possibilities for low-cost and large-scale production of high-rate Nb<sub>2</sub>O<sub>5</sub> for sodium-storage applications.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.15","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138454682","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrocatalytic conversion of waste polyamide-66 hydrolysates into high-added-value adiponitrile and hydrogen fuel 废聚酰胺-66水解物电催化转化为高附加值己二腈和氢燃料
Electron Pub Date : 2023-11-23 DOI: 10.1002/elt2.14
Chuqian Xiao, Wan Ru Leow, Luyang Chen, Yuhang Li, Chunzhong Li
{"title":"Electrocatalytic conversion of waste polyamide-66 hydrolysates into high-added-value adiponitrile and hydrogen fuel","authors":"Chuqian Xiao,&nbsp;Wan Ru Leow,&nbsp;Luyang Chen,&nbsp;Yuhang Li,&nbsp;Chunzhong Li","doi":"10.1002/elt2.14","DOIUrl":"https://doi.org/10.1002/elt2.14","url":null,"abstract":"<p>To reduce environmental pollution and plastic recycling costs, polyamide-66 (PA-66) as the most consumed engineering polymer needs to be recycled effectively. However, the existing recycling methods cannot convert waste PA-66 into valuable chemicals for upcycling under ambient conditions. Here, we report an integrated hydrolysis and electrocatalytic process to upcycle waste PA-66 into valuable adiponitrile (ADN), adipic acid, and H<sub>2</sub> commodities, thereby closing the PA-66 loop. To enable electrooxidation of the PA-66 hydrosylate hexamethylenediamine (HMD), we fabricated anode catalysts with hierarchical Ni<sub>3</sub>S<sub>2</sub>@Fe<sub>2</sub>O<sub>3</sub> core-shell heterostructures comprising spindle-shaped Ni<sub>3</sub>S<sub>2</sub> cores and Fe<sub>2</sub>O<sub>3</sub> nanosheet shells. The unique core-shell architecture and synergy of the Ni<sub>3</sub>S<sub>2</sub> and Fe<sub>2</sub>O<sub>3</sub> catalysts enabled the selective dehydrogenation of C–N bonds from HMD to nitrile C≡N bonds, forming ADN with near-unity Faradaic efficiency at 1.40 V during the 100-h stability test even at 100 mA cm<sup>−2</sup>. X-ray photoelectron spectroscopy revealed that the Ni(Fe) oxy(hydroxide) species formed were in the active state during oxidation, accelerating the activation of the amino C–N bond for dehydrogenation directly into the C≡N bonds.</p>","PeriodicalId":100403,"journal":{"name":"Electron","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elt2.14","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138454683","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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