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Materials Today Catalysis Pub Date : 2025-03-01 DOI: 10.1016/S2949-754X(25)00009-2
{"title":"Ediorial Board","authors":"","doi":"10.1016/S2949-754X(25)00009-2","DOIUrl":"10.1016/S2949-754X(25)00009-2","url":null,"abstract":"","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100096"},"PeriodicalIF":0.0,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143628376","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
Facile one-pot surfactant-free synthesis of 3D vertical graphene anchored ultrafine PtCo nanoparticles for ethanol oxidation 一锅无表面活性剂的3D垂直石墨烯锚定超细PtCo纳米颗粒乙醇氧化合成
Materials Today Catalysis Pub Date : 2025-03-01 DOI: 10.1016/j.mtcata.2025.100094
Mingxing Nie , Fengyi Liu , Zijian Wang , Wei Gan , Jie Yu , Bin Wu , Qunhui Yuan
{"title":"Facile one-pot surfactant-free synthesis of 3D vertical graphene anchored ultrafine PtCo nanoparticles for ethanol oxidation","authors":"Mingxing Nie ,&nbsp;Fengyi Liu ,&nbsp;Zijian Wang ,&nbsp;Wei Gan ,&nbsp;Jie Yu ,&nbsp;Bin Wu ,&nbsp;Qunhui Yuan","doi":"10.1016/j.mtcata.2025.100094","DOIUrl":"10.1016/j.mtcata.2025.100094","url":null,"abstract":"<div><div>Exploring highly active catalysts with high Pt utilization rates is still challenging for direct ethanol fuel cells (DFECs). Herein, we report a facile synthesis of three-dimensional (3D) vertical graphene (VG) supported PtCo alloy nanoparticles (PtCo/VG) as catalysts for ethanol oxidation reactions (EOR). The 3D interconnected open network and exposed edges of VG nanosheets provide an ideal support for hindering the aggregation of PtCo nanoparticles and thus the PtCo nanoparticles achieve an ultrasmall size of 3.7 nm and a high dispersion on VG supports. PtCo/VG displays a superb mass activity (4.33 A mg<sup>−1</sup>) and specific activity (5.14 mA cm<sup>−2</sup>) toward EOR, which are 5.6 and 3.5 times to those of commercial Pt/C, respectively. The catalytic activity of PtCo/VG also surpasses its counterparts of carbon fibers supported PtCo (PtCo/CNFs) and XC-72 supported PtCo (PtCo/XC-72), and behaves amazingly among many reported Pt-based catalysts. Density functional theory (DFT) calculations demonstrate that the introduction of VG supports lowered the Pt d-band center, weakened the CO adsorption and strengthened the OH adsorption on catalytic sites of PtCo/VG. This work may pave the way for fabricating highly carbon-based efficient bifunctional electrocatalysts with high platinum utilization for fuel cells.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100094"},"PeriodicalIF":0.0,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143578379","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 synthesis of pure H2O2 from crossover oxygen through a porous proton exchange membrane 通过多孔质子交换膜由交叉氧电催化合成纯H2O2
Materials Today Catalysis Pub Date : 2025-03-01 DOI: 10.1016/j.mtcata.2025.100088
Kazuma Enomoto, Takuya Okazaki, Kosuke Beppu, Fumiaki Amano
{"title":"Electrocatalytic synthesis of pure H2O2 from crossover oxygen through a porous proton exchange membrane","authors":"Kazuma Enomoto,&nbsp;Takuya Okazaki,&nbsp;Kosuke Beppu,&nbsp;Fumiaki Amano","doi":"10.1016/j.mtcata.2025.100088","DOIUrl":"10.1016/j.mtcata.2025.100088","url":null,"abstract":"<div><div>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a valuable chemical, and its eco-friendly electrochemical production has gained attention to obtain pH-neutral aqueous solutions without impurities. However, achieving H<sub>2</sub>O<sub>2</sub> faradaic efficiencies (FEs) above 30 % has been a challenge with conventional proton exchange membrane (PEM) electrolyzers. To enhance H<sub>2</sub>O<sub>2</sub> FE, efficient collection of H<sub>2</sub>O<sub>2</sub> from the catalyst surface using liquid water is necessary, but oxygen diffusion becomes a limiting factor in aqueous-immersed systems. To overcome this, we designed a zero-gap electrolyzer, supplying oxygen gas from the anode side through the membrane to the cathode. A gas flow-through porous PEM was developed by embedding an acidic ionomer into a membrane filter, enabling the crossover oxygen supply to the cathode flooded with water. This porous PEM design facilitated the formation of a three-phase interface at the catalyst, where high-concentration oxygen gas and liquid water interact closely, achieving 79 % H<sub>2</sub>O<sub>2</sub> FE at 5 mA cm<sup>−2</sup>. Continuous synthesis of pure H<sub>2</sub>O<sub>2</sub> solution exceeding 5500 mg L<sup>−1</sup> (0.55 wt%) was sustained for over 50 hours.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100088"},"PeriodicalIF":0.0,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143628382","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 封面
Materials Today Catalysis Pub Date : 2025-03-01 DOI: 10.1016/S2949-754X(25)00008-0
{"title":"Cover","authors":"","doi":"10.1016/S2949-754X(25)00008-0","DOIUrl":"10.1016/S2949-754X(25)00008-0","url":null,"abstract":"","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100095"},"PeriodicalIF":0.0,"publicationDate":"2025-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143628375","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
Facet engineering of Weyl semimetals for efficient hydrogen evolution reaction 用于高效析氢反应的Weyl半金属表面工程
Materials Today Catalysis Pub Date : 2025-02-10 DOI: 10.1016/j.mtcata.2025.100091
Ting Wai Lau , Qiong Lei , Jun Yin
{"title":"Facet engineering of Weyl semimetals for efficient hydrogen evolution reaction","authors":"Ting Wai Lau ,&nbsp;Qiong Lei ,&nbsp;Jun Yin","doi":"10.1016/j.mtcata.2025.100091","DOIUrl":"10.1016/j.mtcata.2025.100091","url":null,"abstract":"<div><div>The design of highly efficient hydrogen evolution reaction (HER) catalysts is a critical challenge in advancing electrochemical water splitting for renewable energy applications. Topological semimetals have recently emerged as promising candidates for HER catalysis; however, the relationship between their topological surface properties and catalytic performance remains poorly understood. Herein, we employ density functional theory (DFT) calculations to investigate the impact of facets on the HER activity of topological TaAs semimetal family (TaAs, NbP, NbAs, and TaP). Our results reveal that topological surface states persist across various facets, and facets with lower coordination numbers exhibit greater stability. Four key theoretical descriptors—Gibbs free energy changes, surface energy, energy barriers for water dissociation, and water adsorption energy—are assessed to provide a comprehensive evaluation of HER activity. For all four compounds, (111) and metal-rich (001) facets exhibit optimal energy values across these metrics, outperforming the benchmark Pt (111). The number of Fermi arcs is found to have a minimal influence on HER activity. Changes in the projected density of states (PDOS) of surface atoms strongly correlate with Δ<em>G</em><sub>H*</sub>, serving as a more effective indicator of HER activity. These findings highlight the importance of a holistic evaluation framework that extends beyond Gibbs free energy changes alone, incorporating multiple factors to identify high-performance catalysts. This work provides new insights into the design principles for topological catalysts in HER and offers valuable guidance for developing next generation of electrocatalysts.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100091"},"PeriodicalIF":0.0,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143420339","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
Coupling cobalt single-atom catalyst with recyclable LiBr redox mediator enables stable LiOH-based Li-O2 batteries 偶联钴单原子催化剂与可回收的LiBr氧化还原介质可以实现稳定的lioh基Li-O2电池
Materials Today Catalysis Pub Date : 2025-02-07 DOI: 10.1016/j.mtcata.2025.100090
Kang Huang , Zhixiu Lu , Shilong Dai , Chunyu Cui , Nam Dong Kim , Huilong Fei
{"title":"Coupling cobalt single-atom catalyst with recyclable LiBr redox mediator enables stable LiOH-based Li-O2 batteries","authors":"Kang Huang ,&nbsp;Zhixiu Lu ,&nbsp;Shilong Dai ,&nbsp;Chunyu Cui ,&nbsp;Nam Dong Kim ,&nbsp;Huilong Fei","doi":"10.1016/j.mtcata.2025.100090","DOIUrl":"10.1016/j.mtcata.2025.100090","url":null,"abstract":"<div><div>Cycling Li-O<sub>2</sub> batteries (LOBs) via LiOH is promising for developing practically viable batteries, while promoting the formation and decomposition of LiOH remains a challenge. Cobalt single atom catalysts (Co-SACs) have been exploited to mediate the direct 4e<sup>−</sup> oxygen reduction reaction for generating LiOH discharge products, but their inferior oxygen evolution activity renders the battery low energy efficiency and poor cycling life. Herein, we for the first time introduce LiBr redox mediator (RM) into the Co-SACs-catalyzed LOB system to facilitate the decomposition of LiOH. In the discharge process, the catalysis of Co-SAC is unaffected with the presence of LiBr. During charging, Br<sub>3</sub><sup>−</sup> is identified as the oxidizer to decompose LiOH at an appropriate potential (3.6 V). Significantly, the soluble Br<sup>−</sup>‬‬‬‬‬ is recyclable in the system as the BrO<sup>−</sup> intermediate‬‬‬‬‬‬‬‬‬‬ could shuttle to the anode and react with Li metal to regenerate Br<sup>−</sup>‬‬‬‬‬ ‬‬so that the generation of LiBrO<sub>3</sub> deposit is circumvented‬‬‬‬‬‬‬‬. Consequently, the fabricated LOB demonstrates fewer side reactions, stable energy efficiency (drop rate of 0.10 % per cycle) and long cycle life (300 cycles at 1000 mA/g) under the ambient atmosphere.‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬‬</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100090"},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143378854","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
Modulating selectivity and stability of the direct seawater electrolysis for sustainable green hydrogen production 海水直接电解可持续绿色制氢的选择性和稳定性调控
Materials Today Catalysis Pub Date : 2025-02-06 DOI: 10.1016/j.mtcata.2025.100089
Dazhi Yao , Chun Liu , Yanzhao Zhang , Shuhao Wang , Yan Nie , Man Qiao , Dongdong Zhu
{"title":"Modulating selectivity and stability of the direct seawater electrolysis for sustainable green hydrogen production","authors":"Dazhi Yao ,&nbsp;Chun Liu ,&nbsp;Yanzhao Zhang ,&nbsp;Shuhao Wang ,&nbsp;Yan Nie ,&nbsp;Man Qiao ,&nbsp;Dongdong Zhu","doi":"10.1016/j.mtcata.2025.100089","DOIUrl":"10.1016/j.mtcata.2025.100089","url":null,"abstract":"<div><div>Direct seawater electrolysis (DSE) has emerged as a compelling route to sustainable hydrogen production, leveraging the vast global reserves of seawater. However, the inherently complex composition of seawater—laden with halide ions, multivalent cations (Mg<sup>2</sup><sup>+</sup>, Ca<sup>2+</sup>), and organic/biological impurities—presents formidable challenges in maintaining both selectivity and durability. Chief among these obstacles is mitigating chloride corrosion and suppressing chlorine evolution reaction (ClER) at the anode, while also preventing the precipitation of magnesium and calcium hydroxides at the cathode. This review consolidates recent advances in material engineering and cell design strategies aimed at controlling undesired side reactions, enhancing electrode stability, and maximizing energy efficiency in DSE. We first outline the fundamental thermodynamic and kinetic hurdles introduced by Cl<sup>−</sup> and other impurities. This discussion highlights how these factors accelerate catalyst degradation and drive suboptimal reaction pathways. We then delve into innovative approaches to improve selectivity and durability of DSE—such as engineering protective barrier layers, tuning electrolyte interfaces, developing corrosion-resistant materials, and techniques to minimize Mg/Ca-related precipitations. Finally, we explore emerging reactor configurations, including asymmetric and membrane-free electrolyzers, which address some barriers for DSE commercialization. Collectively, these insights provide a framework for designing next-generation DSE systems, which can achieve large-scale, cost-effective, and environmentally benign hydrogen production.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100089"},"PeriodicalIF":0.0,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143429658","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
Oxygen vacancy-mediated high-entropy oxide electrocatalysts for efficient oxygen evolution reaction 氧空位介导的高效析氧反应的高熵氧化物电催化剂
Materials Today Catalysis Pub Date : 2024-12-31 DOI: 10.1016/j.mtcata.2024.100086
Ruonan Liu , Yaotian Yan , Liang Dun , Taili Yang , Bin Qin , Peijia Wang , Wei Cai , Shude Liu , Xiaohang Zheng
{"title":"Oxygen vacancy-mediated high-entropy oxide electrocatalysts for efficient oxygen evolution reaction","authors":"Ruonan Liu ,&nbsp;Yaotian Yan ,&nbsp;Liang Dun ,&nbsp;Taili Yang ,&nbsp;Bin Qin ,&nbsp;Peijia Wang ,&nbsp;Wei Cai ,&nbsp;Shude Liu ,&nbsp;Xiaohang Zheng","doi":"10.1016/j.mtcata.2024.100086","DOIUrl":"10.1016/j.mtcata.2024.100086","url":null,"abstract":"<div><div>Transition metal oxides hold great potential for water splitting due to their tunable electronic structures and abundant availability. However, their inherently poor electrical conductivity and limited catalytic activity hinder their practical implementation. Herein, high-entropy oxide (FeCoNiCrCuO) electrocatalysts featuring grain-like structure and oxygen vacancies-enriched surface were synthesized through an ultra-fast non-equilibrium high-temperature shock. The introduction of oxygen vacancies modulates the electronic structure and increases the carrier concentration, accelerating the rate-determining step of the oxygen evolution reactions and reducing the overpotential of oxygen evolution reactions. Consequently, the synthesized FeCoNiCrCuO electrocatalyst delivers a low overpotential of 256 mV at a current density of 10 mA·cm⁻² and a Tafel slope of 48.2 mV·dec⁻¹ in 1 M KOH, which is superior to samples lacking oxygen vacancies after annealing. This study presents an alternative approach to enhancing OER activity by employing a high-entropy oxide engineering strategy.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100086"},"PeriodicalIF":0.0,"publicationDate":"2024-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149469","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
Multilayered molybdenum carbonitride MXene: Reductive defunctionalization, thermal stability, and catalysis of ammonia synthesis and decomposition 多层碳氮化钼MXene:还原解功能化、热稳定性及催化氨合成与分解
Materials Today Catalysis Pub Date : 2024-12-27 DOI: 10.1016/j.mtcata.2024.100085
Evgenia Kountoupi , Diana Piankova , Mikhail Agrachev , Zixuan Chen , Alberto Garbujo , Paula M. Abdala , Christoph R. Müller , Alexey Fedorov
{"title":"Multilayered molybdenum carbonitride MXene: Reductive defunctionalization, thermal stability, and catalysis of ammonia synthesis and decomposition","authors":"Evgenia Kountoupi ,&nbsp;Diana Piankova ,&nbsp;Mikhail Agrachev ,&nbsp;Zixuan Chen ,&nbsp;Alberto Garbujo ,&nbsp;Paula M. Abdala ,&nbsp;Christoph R. Müller ,&nbsp;Alexey Fedorov","doi":"10.1016/j.mtcata.2024.100085","DOIUrl":"10.1016/j.mtcata.2024.100085","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Harnessing two-dimensional (2D) materials for catalytic applications is promising due to the high site utilization. Here, we synthesized a 2D molybdenum carbonitride of the MXene family, Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt;, and applied it as a catalyst for ammonia synthesis and decomposition, the essential reactions to establish NH&lt;sub&gt;3&lt;/sub&gt; as an energy vector. We determine the thermal stability limit of Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; under H&lt;sub&gt;2&lt;/sub&gt; flow to be ca. 575 °C. Exceeding this temperature results, under H&lt;sub&gt;2&lt;/sub&gt;, in a transformation of the predominantly defunctionalized Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; to a 3D Mo&lt;sub&gt;2&lt;/sub&gt;(C,N) phase, which prevents the complete defunctionalization of Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; while retaining its 2D morphology. Before this phase transformation occurs, the remaining &lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; species reside in the interior layers of the mostly defunctionalized Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; nanoplatelets, with the amorphous exterior being free from &lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; groups, rendering the Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; nanoplatelets chemically anisotropic in the direction orthogonal to the basal plane. The effect of this structure on catalytic properties is highlighted in the thermocatalytic synthesis and decomposition of NH&lt;sub&gt;3&lt;/sub&gt;. In the latter reaction, Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; shows similar gravimetric rates to a reference bulk β-Μο&lt;sub&gt;2&lt;/sub&gt;Ν catalyst, which is ascribed to the presence of too narrow 2D pores (ca. 5.2 Å) with irregular shapes due to a disorder in the stacking of nanosheets in Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt;, limiting interlayer diffusion. A deactivation pathway in Mo-based MXenes was identified, and it relates to a precipitation of carbon vacancies to metallic molybdenum under NH&lt;sub&gt;3&lt;/sub&gt; decomposition conditions. While the ammonia decomposition reaction shows no dependence of the reaction rate on the specific H&lt;sub&gt;2&lt;/sub&gt; pretreatment of Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; (500 or 575 °C), the gravimetric ammonia formation rate increases appreciably with H&lt;sub&gt;2&lt;/sub&gt; pretreatment, &lt;em&gt;viz&lt;/em&gt;., Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; pretreated at 575 °C outperforms by ca. four times both the reference β-Μο&lt;sub&gt;2&lt;/sub&gt;Ν catalyst and Mo&lt;sub&gt;2&lt;/sub&gt;(C,N)&lt;em&gt;T&lt;/em&gt;&lt;sub&gt;&lt;em&gt;x&lt;/em&gt;&lt;/sub&gt; pretreated at 500 °C, explained by a smaller molecule size of the reactants H&lt;sub&gt;2&lt;/sub&gt; and N&lt;sub&gt;2&lt;/sub&gt; relative to NH&lt;sub&gt;3&lt;/sub&gt;, and an increased accessibility and utilization of the interlayer space for ammonia synthesis. Overall, our study highlights the importance of addressing limitations due to small pore sizes in multilayered MXenes and the stability of carbon vacancies while simultaneously using optimized pretreatment conditions for surface defunctio","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100085"},"PeriodicalIF":0.0,"publicationDate":"2024-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143149470","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
Boosting oxygen evolution of LiCoO2 electrocatalysts via lithium defect 锂缺陷对LiCoO2电催化剂析氧性能的影响
Materials Today Catalysis Pub Date : 2024-12-25 DOI: 10.1016/j.mtcata.2024.100087
Huamei Li , Mengyuan Li , Lingling Liao , Han Yang , Kun Xiang , Guoqiang Luo , Mingjiang Xie
{"title":"Boosting oxygen evolution of LiCoO2 electrocatalysts via lithium defect","authors":"Huamei Li ,&nbsp;Mengyuan Li ,&nbsp;Lingling Liao ,&nbsp;Han Yang ,&nbsp;Kun Xiang ,&nbsp;Guoqiang Luo ,&nbsp;Mingjiang Xie","doi":"10.1016/j.mtcata.2024.100087","DOIUrl":"10.1016/j.mtcata.2024.100087","url":null,"abstract":"<div><div>The challenge of the complex oxygen evolution reaction (OER) currently impedes the efficient production of hydrogen via electrolytic water splitting. To address this issue, the development and improvement of effective electrocatalysts are required. LiCoO<sub>2</sub>, a key material in lithium-ion batteries, has shown promising potential as an electrocatalyst for electrochemical energy conversion. However, OER catalysts derived from LiCoO<sub>2</sub> have faced obstacles such as high overpotential and a complicated preparation process. In this study, the preparation method is adjusted to optimize the synthesis of Li<sub>1-x</sub>CoO<sub>2</sub> with a defective structure, resulting in an impressive overpotential of only 290 mV at a current density of 100 mA cm<sup>−2</sup> and a remarkable Tafel slope of 15.2 mV dec<sup>−1</sup>. The exceptional catalytic activity of Li<sub>1-x</sub>CoO<sub>2</sub> can be attributed to the absence of Li, which triggers oxidative alterations in the electronic structure of Co. Density functional theory (DFT) calculations reveal that Li defects can influence the d-band center of active Co sites, enhancing the adsorption capabilities of Co sites towards *OOH intermediates and increasing the conductivity of the electrocatalyst during the OER process. These alterations improve the velocity of the crucial step in the reaction, ultimately boosting the catalyst's overall performance and efficiency.</div></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"8 ","pages":"Article 100087"},"PeriodicalIF":0.0,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143148539","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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