Journal of Materials Chemistry A最新文献_第8页

Synergistic hydrazine-driven regulation and Mo/S co-doping to endow BiOBr with heterovalent molybdenum states and abundant oxygen vacancy defects for photocatalytic hydrogen evolution 肼驱动的协同调节和 Mo/S 共掺杂使 BiOBr 具有异价钼态和丰富的氧空位缺陷，从而实现光催化氢气进化

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-20 DOI: 10.1039/d4ta05641h

Zhengjie Su, Binghong Wu, Dong-Hau Kuo, Longyan Chen, Pengkun Zhang, Baoqian Yang, Xinru Wu, Dong fang Lu, Jinguo Lin, Xiaoyun Chen

{"title":"Synergistic hydrazine-driven regulation and Mo/S co-doping to endow BiOBr with heterovalent molybdenum states and abundant oxygen vacancy defects for photocatalytic hydrogen evolution","authors":"Zhengjie Su, Binghong Wu, Dong-Hau Kuo, Longyan Chen, Pengkun Zhang, Baoqian Yang, Xinru Wu, Dong fang Lu, Jinguo Lin, Xiaoyun Chen","doi":"10.1039/d4ta05641h","DOIUrl":"https://doi.org/10.1039/d4ta05641h","url":null,"abstract":"Herein, we demonstrate a Mo/S co-doped BiOBr-based bimetal bismuth sulfur-oxybromide (Mo/S-BiOBr) catalyst with heterovalent molybdenum states and abundant oxygen vacancy defects for photocatalytic hydrogen evolution (PHER) via a facile method. Mo/S co-doping adjusts the energy band structure of BiOBr and expands the visible light absorption. The hydrazine regulates the molybdenum with heterovalent states while endows Mo/S-BiOBr with oxygen vacancy defects to balance the valence-charge deviations from electrical neutrality induced by Mo6+→Mo4+. These oxygen-vacancy defects act as active sites for capturing water molecules and activating the H-O-H bond to produce protons for hydrogen generation. The heterovalent Mo6+/Mo4+ states act as photogenerated electron hosts to hop fast between Mo6+ and Mo4+, facilitating efficient electron transfer for PHER. The hybridization between S3p and O2p orbital improves the stability of continuous PHER. The hydrazine-regulated Mo/S-BiOBr-3 with an optimal n(Mo4+)/n(Mo4+ + Mo6+) ratio and abundant oxygen vacancy defects exhibits excellent PHER activity of 710.5 µmol·h−1 at the catalyst weight of 50 mg and an apparent quantum efficiency (AQE) of 13.9% at 420 nm. After six recycles, the H2 yield of Mo/S-BiOBr-3 decreased by only about 3.5%, indicating good stability and durability. This work provides a practical approach to using bismuth-based oxyhalides in PHER.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247268","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Highly stretchable ionic hydrogels with enhanced thermoelectric performance and flame retardancy for intelligent fire protection 可高度拉伸的离子水凝胶，具有增强的热电性能和阻燃性能，可用于智能防火系统

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-20 DOI: 10.1039/d4ta05396f

Mi Fu, Zhengzhong Wu, Xiaobo Liu, Yuwei Yuan, Xuejun Lai, Kan Yue

{"title":"Highly stretchable ionic hydrogels with enhanced thermoelectric performance and flame retardancy for intelligent fire protection","authors":"Mi Fu, Zhengzhong Wu, Xiaobo Liu, Yuwei Yuan, Xuejun Lai, Kan Yue","doi":"10.1039/d4ta05396f","DOIUrl":"https://doi.org/10.1039/d4ta05396f","url":null,"abstract":"Fire disasters pose a significant threat to life and property worldwide, underscoring the urgent necessity for advanced fire prevention technologies. In the field of intelligent fire protection materials, thermoelectric fire-resistant materials have garnered considerable attention due to their high sensitivity and the distinct advantage of not requiring an external power supply. This feature endows them with high responsiveness and energy efficiency in detecting and responding to fire incidents, thereby enhancing overall safety measures. In this study, we develop a series of highly stretchable ionic hydrogels with exceptional thermoelectric properties and flame retardancy for intelligent fire protection applications. Through a simple one-pot photopolymerization process, polyacrylic acid (PAA) and polyethylene glycol (PEO) were combined with sodium dihydrogen phosphate (SDP) to form a robust hydrogen-bonded ionic hydrogel network. The resulting PAA-PEO-SDP ionic hydrogels demonstrated an impressive elongation at break up to 4270% and a very high ionic Seebeck coefficient of 24.7 mV K−1. The incorporation of the phosphorus salt enhanced flame retardancy to reach the UL-94 V-0 rating and significantly increased the oxygen index of encapsulated wood from 27% to 54%. Moreover, as a fire-warning device, it could rapidly generate an output voltage of ca. 50 mV within 1.5 s upon exposure to fire, showcasing potential for autonomous fire prevention systems. This work highlights the synergistic integration of mechanical flexibility, thermoelectric performance, and fire safety in the development of next-generation intelligent materials for fire protection.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Single-Crystalline High-Entropy Oxide Particles Synthesized via Coordination Polymerization 通过配位聚合合成的单晶高熵氧化物粒子

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-20 DOI: 10.1039/d4ta05218h

Yuguang Pu, Zhen He, Jiaming Liu, Tingxuan Yang, Hongliang Zhang, Saifang Huang, Hong Zhang, Wen Zhang, Tianzu Yang, Puqi Jia, Wei Gao, Peng Cao

{"title":"Single-Crystalline High-Entropy Oxide Particles Synthesized via Coordination Polymerization","authors":"Yuguang Pu, Zhen He, Jiaming Liu, Tingxuan Yang, Hongliang Zhang, Saifang Huang, Hong Zhang, Wen Zhang, Tianzu Yang, Puqi Jia, Wei Gao, Peng Cao","doi":"10.1039/d4ta05218h","DOIUrl":"https://doi.org/10.1039/d4ta05218h","url":null,"abstract":"High-entropy oxides (HEOs) have attracted increasing attention due to their extreme chemical disorder incorporated in long-range structural order. Various single-phase HEOs have been successfully fabricated through solid-state synthesis, yet the resulting materials are often bulky aggregates. Solution-based chemical reactions can be applied to prepare HEO particles. However, the co-precipitation of multiple metal ions is practically challenging, given that the composition of a precipitated HEO can deviate significantly from an equimolar ratio. Here, coordination polymerization has been coupled with solid dispersant-assisted annealing, producing single-crystalline HEO rods with uniform dispersion. The stepwise polymerization of cations into metal-organic chains (MOCs) enables homogeneous deposition of different metals into submicron-sized particles. Owing to this pre-mixing feature of oxalate precursors, single-phase HEOs can be obtained through short annealing. While this deposition method extends the compositional spectrum of rocksalt HEO to other metals and simplifies the production of HEO particles with single-crystalline structures, solid dispersants enable the retention of the morphology and dispersity of precursor particles after annealing. The resulting HEO single crystals demonstrate impressive cycle performance in half-cell and full-cell configurations.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Pyrenetetrayl/phenanthroline-based one-dimensional covalent organic framework for metal-free photocatalytic organic conversion 用于无金属光催化有机转换的基于吡咯烷酮/菲罗啉的一维共价有机框架

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta04330h

Longfei Wang, Longxin Wang, Qianrui Zhao, Xiaoming Ji, Mingqin Zhao, Yujie Zhang, Miao Lai

{"title":"Pyrenetetrayl/phenanthroline-based one-dimensional covalent organic framework for metal-free photocatalytic organic conversion","authors":"Longfei Wang, Longxin Wang, Qianrui Zhao, Xiaoming Ji, Mingqin Zhao, Yujie Zhang, Miao Lai","doi":"10.1039/d4ta04330h","DOIUrl":"https://doi.org/10.1039/d4ta04330h","url":null,"abstract":"Covalent organic frameworks (COFs) are a new type of metal-free heterogeneous catalysts that have emerged recently and are often used in light-driven organic transformations. Nevertheless, the photocatalytic organic conversion is predominantly based on 2D or 3D topological structures, leaving 1D topology of COFs relatively unexplored systematically in this field. Herein, a one-dimensional phenanthroline-based covalent organic framework, named PP-COF, was developed by combining 4,4',4'',4'''-(1,3,6,8-pyrenetetrayl) tetrakis[benzenamine] (PTBA) and 4,4'-(1,10-phenanthroline-2,9-diyl) bis[benzaldehyde] (PBBA). The prepared PP-COF not only possesses a high crystallinity, and remarkable stability, but also exhibits excellent light absorption capabilities within the visible-light range and favorable photoelectric response characteristics, compared to 2D PyTTA-COF. PP-COF can efficiently convert O2 to 1O2 and O2•− by exposure to air and visible light. This in turn facilitates the photocatalytic indoles functionalization and oxidative thiols coupling to yield bisaryl indoles and disulfides in yields ranging from moderate to high, respectively. Furthermore, the PP-COF exhibits excellent recyclability. This study proposes that the potential for light-induced organic conversion is promising in one-dimensional linear covalent organic frameworks.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245908","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ni–P codoping engineered MoS2 basal planes for electrocatalytic water splitting: Insights from density functional theory 用于电催化水分离的 Ni-P 共掺工程 MoS2 基底面：密度泛函理论的启示

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta04025b

Le Thanh Phuong, Sampath Prabhakaran, Do Hwan Kim

{"title":"Ni–P codoping engineered MoS2 basal planes for electrocatalytic water splitting: Insights from density functional theory","authors":"Le Thanh Phuong, Sampath Prabhakaran, Do Hwan Kim","doi":"10.1039/d4ta04025b","DOIUrl":"https://doi.org/10.1039/d4ta04025b","url":null,"abstract":"The development of efficient bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in water splitting is crucial for clean energy generation. This study investigated the potential of substitutional heteroatom doping in metallic 1T-phase MoS2 monolayers (MLs) using first-principles calculations. Ni and P codoping significantly improved the electrical conductivity and active site reactivity of the distorted 1T-MoS2 lattice. Doping modulated the electronic band structure, inducing spin-polarized states with enhanced d-band conductivity near the Fermi level. This manipulation, governed by the altered valence and conduction bands, also facilitated efficient charge transfer and reduced interfacial resistance. Furthermore, the strong dopant promoted the adsorption behavior at various active sites on the surface, lowering the Gibbs free energy for the HER (0.083 eV) and decreasing the OER overpotential (0.39 V). Therefore, the heteroatom doping of 1T-MoS2 MLs is a powerful strategy for developing advanced and low-cost electrocatalysts that can accelerate water splitting and operate without platinum.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245667","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Artificial CO2 photoreduction: a review of photocatalyst design and product selectivity regulation 人工二氧化碳光还原：光催化剂设计和产品选择性调节综述

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta04600e

Chen Fu, Zhenyu Wan, Xin Yang, Junhui Zhang, Zizhong Zhang

{"title":"Artificial CO2 photoreduction: a review of photocatalyst design and product selectivity regulation","authors":"Chen Fu, Zhenyu Wan, Xin Yang, Junhui Zhang, Zizhong Zhang","doi":"10.1039/d4ta04600e","DOIUrl":"https://doi.org/10.1039/d4ta04600e","url":null,"abstract":"Mimicking the natural photosynthesis, artificial photosynthesis of CO2 reduction into valuable hydrocarbon fuels is a promising approach to solar energy utilizatio and carbon neutrality. However, great challenges are present in the development of an efficient photocatalyst for CO2 reduction and the controlling of the selectivity of reduction products. This review summarizes the progress of photocatalyst design strategies to improve the efficiency and selectivity of photocatalytic CO2 reduction. Six popular modification methods are introduced, such as defect structure, cocatalst loading, doping heterojunction formation, single atom engineering, and surface organometallics catalysis. The effects of different strategies on the promotion of light absorption, charge separation and migration and catalyst surface reaction in the process of O2 reduction are analyzed. In addition, the latest research results of selective reduction to C1, C2, and C2+ in CO2 and H2O systems are summarized. Finally, the article delves into the future prospects and inherent hurdles in photocatalyst design with a focus on enhancing the selectivity of CO2 conversion towards specific products. This review provides an insight of the efficiency and selectivity in photocatalytic CO2 reduction across various photocatalysts, thereby serving as a a valuable guidance for the advancement of high-performance photocatalyst.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245664","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Nanoarchitectured 2D-2D Heterointerface of Pt@Ti3C2Tx-rGO Aerogels via In-Situ γ-Radiolysis Induced Self-Assembly: Interplay between Strain and Ligand Effects in Electrocatalytic Interfaces 通过原位 γ 辐射诱导自组装实现 Pt@Ti3C2Tx-rGO 气凝胶的纳米结构 2D-2D 异质界面：电催化界面中应变和配体效应的相互作用

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta02688h

Linsha Vazhayal, Sharon Benny Alex, Santosh Haram

{"title":"Nanoarchitectured 2D-2D Heterointerface of Pt@Ti3C2Tx-rGO Aerogels via In-Situ γ-Radiolysis Induced Self-Assembly: Interplay between Strain and Ligand Effects in Electrocatalytic Interfaces","authors":"Linsha Vazhayal, Sharon Benny Alex, Santosh Haram","doi":"10.1039/d4ta02688h","DOIUrl":"https://doi.org/10.1039/d4ta02688h","url":null,"abstract":"Achieving high-performance and cost-effective Pt-based catalysts with low Pt content and thereby boosting Pt utilization remains a significant challenge in the field of oxygen and hydrogen electrocatalysis. The authentic performance of Pt is often hindered by the occupancy and poisoning of active sites, weak Pt support interaction, and the degradation of catalyst. To address these issues, we demonstrate a rational design of low Pt loaded 3D porous aerogel support through self-assembly and reduction of a 2D-2D heterostructure comprising MXene (Ti3C2Tx) and reduced graphene oxide (rGO) via γ-radiolytic synthesis process. The aerogel heterointerface effectively prevents Ti3C2Tx restacking and aggregation, thereby enhancing the interaction of electrocatalyst with electrolyte. Through precise regulation of the heterojunction interface with a strong metal support interaction (SMSI), Pt@Ti3C2Tx-rGO catalyst demonstrates excellent electrocatalytic performance for HER, OER, and ORR. Pt@ Ti3C2Tx-rGO catalyst exhibits efficient ORR activity, with a high onset-potential of 0.957 V, and a low overpotentials for the HER (43 mV) and OER (490 mV) at current density 10 mA cm−2, as well as excellent stability against degradation in an acidic condition. Furthermore, we studied the role of the electronic effects (ligand and strain) induced by SMSI. Spectroscopic analysis confirms that the observed downward shift in the Pt d-band center, is attributed to both charge transfer from the support to Pt and compressive strain exerted on the Pt lattice, is responsible for the enhanced electrocatalytic activity. This work successfully offers strategic guidance for charge transfer and strain equilibration in heterointerface toward the rational design of advanced electrocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Regulating from Local Electron Density to Adsorption Energy of COF-based Single Copper Sites for Highly Efficient Fenton-like Photo-oxidation 从局部电子密度到 COF 基单铜位点吸附能的调节，实现高效芬顿样光氧化反应

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta04418e

Qianqian Peng, Guijiao Wen, Chen Yuan, Caizhi Lv, Lan Wu, Juan He, Xiandeng Hou

{"title":"Regulating from Local Electron Density to Adsorption Energy of COF-based Single Copper Sites for Highly Efficient Fenton-like Photo-oxidation","authors":"Qianqian Peng, Guijiao Wen, Chen Yuan, Caizhi Lv, Lan Wu, Juan He, Xiandeng Hou","doi":"10.1039/d4ta04418e","DOIUrl":"https://doi.org/10.1039/d4ta04418e","url":null,"abstract":"Highly efficient single-atom catalysts (SACs) hold great potential for promoting peroxymonosulfate (PMS) activation to facilitate organic pollutant degradation but remain a challenge to precisely regulate and enhance their catalytic efficiency. Here, single Cu atom catalysts anchored on a series of ketoenamine-based covalent organic frameworks (COFs) were developed as PMS activators via a facile dielectric barrier discharge (DBD) plasma and wet chemical method. Based on the systematic engineering of photoelectric structure at the molecular level, the charge distribution was precisely regulated by introducing different functional groups (Cu@TpPa-X, X= -(CH3)2, -H, -CN). Among the obtained materials, Cu@TpPa-(CH3)2 possesses the best photocatalytic capability, the mineralization (90%) of carbamazepine (CBZ) and the reaction rate constant (0.322 min-1) are comparable to those of the most advanced photocatalysts. Experiments and calculations demonstrate that the introduction of individual metal atoms increases the electron density at the active center, and electron-donating groups accelerate the transfer of photogenerated carriers and improve the PMS adsorption to the material, which significantly improves the overall oxidation and mineralization kinetics. This work pioneers a novel approach for tailoring high-efficiency COFs-based SACs, thus broadening their potential applications in photo-catalysis.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245958","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual Single-Atom Sites Coupled with Graphene-Encapsulated Core-Shell Fe-Cu Nanoalloy for Boosting Oxygen Reduction Reaction 与石墨烯封装的核壳铁铜纳米合金耦合的双单原子位点用于促进氧还原反应

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta05015k

Katam Srinivas, Zhou Chen, Anran Chen, He Huang, Chengtao Yang, Fei Wang, Ming-Qiang Zhu, Yuanfu Chen

{"title":"Dual Single-Atom Sites Coupled with Graphene-Encapsulated Core-Shell Fe-Cu Nanoalloy for Boosting Oxygen Reduction Reaction","authors":"Katam Srinivas, Zhou Chen, Anran Chen, He Huang, Chengtao Yang, Fei Wang, Ming-Qiang Zhu, Yuanfu Chen","doi":"10.1039/d4ta05015k","DOIUrl":"https://doi.org/10.1039/d4ta05015k","url":null,"abstract":"Replacing platinum-based electrocatalysts with iron single-atom catalysts (Fe-N4-C) for the oxygen reduction reaction (ORR) remains challenging due to the symmetric electronic structure of atomically dispersed Fe-N4 sites and sluggish kinetics. To address this issue, we introduce Cu-Nx sites and graphene-encapsulated core-shell Fe-Cu nanoalloy (FeCu@G) particles into the Fe-Nx site surroundings through self-assembly and pyrolysis of a metal-organic framework (MOF). This strategy leverages synergistic interactions with the associated species to modify the uniform electronic structure of Fe single-atom sites, thereby enhancing oxygen-adsorption/desorption kinetics. Density functional theory (DFT) calculations reveal that the incorporation of Cu-Nx sites and FeCu@G nanoalloy significantly alters the electronic structure of Fe-Nx sites, leading to improved ORR activity. Consequently, the optimized FeCu-DSAs@CNT, comprising dual single-atom sites (DSAs: Fe-Nx and Cu-Nx) and FeCu@G nanoalloy within MOF-derived nitrogen-doped carbon nanotubes (CNT), exhibits a significantly improved half-wave potential (E1/2 = 0.91 V) and feasible ORR kinetics (Tafel slope = 48.15 mV dec-1), surpassing the Pt/C benchmark (E1/2 = 0.847 V and Tafel slope = 56.76 mV dec-1). Notably, FeCu-DSAs@CNT shows a 58 mV more positive E1/2 compared to monometallic Fe-SAs@CNT, attributed to synergistic interactions with Cu species. Moreover, it demonstrates excellent power density, specific capacity, and cycling stability in a lab-made Zinc-air battery, outpacing the Pt/C-battery. This study addresses gaps in understanding Fe-Nx site interactions with associated species, providing valuable insights for the advancement of Fe-Nx-C electrocatalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142245666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Non-thermal plasma enabled catalytic dry reforming of methane over ceria nanorods supported NiO catalyst: the role of Ru as coke resistant active sites 铈纳米棒支撑的氧化镍催化剂上的非热等离子体催化甲烷干转化：Ru 作为抗焦活性位点的作用

IF 11.9 2区材料科学

Journal of Materials Chemistry A Pub Date : 2024-09-19 DOI: 10.1039/d4ta04141k

Md Robayet Ahasan, Monir Hossain, Ruigang Wang

{"title":"Non-thermal plasma enabled catalytic dry reforming of methane over ceria nanorods supported NiO catalyst: the role of Ru as coke resistant active sites","authors":"Md Robayet Ahasan, Monir Hossain, Ruigang Wang","doi":"10.1039/d4ta04141k","DOIUrl":"https://doi.org/10.1039/d4ta04141k","url":null,"abstract":"This study reports that how a 14 wt% Ni-1 wt% Ru bimetallic catalyst supported on ceria (CeO2) nanorods (NR) synthesized by wet impregnation can offer superior conversion and stability against coking during non-thermal plasma (NTP)-assisted DRM when compared to monometallic Ni or Ru catalysts. The study revealed that when Ru was introduced as a promoter to CeO2 NR supported Ni catalyst, the DRM conversion percentage increased significantly under NTP (CH4: 92% and CO2: 70%) at 450 °C. Unlike thermal catalysis, plasma catalysis resulted in high yield (46% CO and 40% H2), selectivity (62% CO and 42% H2) at 450 °C. Additionally, the durability (60 minutes) of the catalyst also tested at 350 °C. The bimetallic synergy and formation of CeO2 NR supported Ni-O-Ru solid solution is believed to be the main cause of significantly improved CH4 and CO2 conversions. The high coking resistance of CeO2-NR supported Ni-Ru bimetallic catalyst is attributed to three major factors: (1) the role of Ru in weakening the bond between Ni sites and carbon; (2) the higher dispersion of Ni over CeO2 NR surface; and (3) the accessibility of surface and lattice oxygen over CeO2 NR support, which promotes excellent redox properties and carbon oxidation. The proposed non-equilibrium and bimetallic synergy approach paves the way for cost-efficient and durable DRM catalysts for scalable syngas production from two potent greenhouse gases, which could potentially apply to future energy-efficient industrial processes such as producing syngas and other value-added chemicals.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142247242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0