EES catalysis最新文献

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Conversion of diverse post-consumer PVC waste materials to PE via dual catalytic tandem dehydrochlorination–hydrogenation† 通过双催化串联脱氢氯化-氢化将各种消费后聚氯乙烯废料转化为聚乙烯
EES catalysis Pub Date : 2024-06-05 DOI: 10.1039/D4EY00082J
Galahad O’Rourke, Alina Skorynina, Igor Beckers, Sam Van Minnebruggen, Christel Colemonts, Philippe Gabriels, Peter Van der Veken and Dirk De Vos
{"title":"Conversion of diverse post-consumer PVC waste materials to PE via dual catalytic tandem dehydrochlorination–hydrogenation†","authors":"Galahad O’Rourke, Alina Skorynina, Igor Beckers, Sam Van Minnebruggen, Christel Colemonts, Philippe Gabriels, Peter Van der Veken and Dirk De Vos","doi":"10.1039/D4EY00082J","DOIUrl":"10.1039/D4EY00082J","url":null,"abstract":"<p >Chemical recycling of polyvinyl chloride (PVC) waste poses challenges due to its high chloride content and varied additive formulations. We present a dual catalytic system enabling full conversion of post-consumer PVC waste <em>via</em> tandem dehydrochlorination–hydrogenation. Using a ZnCl<small><sub>2</sub></small> catalyst (0.1–0.2 eq.) for dehydrochlorination and a Ru catalyst (1.0 mol%) for hydrogenation, it directly converts PVC into a lower molecular weight polyethylene (PE)-like polymer. It prevents the problematic formation of polyenes and aromatic char during thermal processing. The system tolerates common additives (<em>e.g.</em> plasticisers and Pb-, Zn- and Ca/Zn-based stabilisers) and effectively dechlorinates materials with high inorganic filler content. The method can process PVC materials with a wide range of <em>M</em><small><sub>n</sub></small> values (29 000–120 000 g mol<small><sup>−1</sup></small>). Methyl cyclohexanecarboxylate emerges as a suitable solvent for the tandem reaction, thereby producing 100% dechlorinated products with low molar mass averages (<em>M</em><small><sub>n</sub></small> ∼ 2400 g mol<small><sup>−1</sup></small> and <em>M</em><small><sub>w</sub></small> ∼ 5000 g mol<small><sup>−1</sup></small>) and allows additive removal. X-ray absorption spectroscopy (XAS) and a study of the reactivity of a model compound elucidate the Ru-catalyst structure and the chain splitting mechanism. This tandem process yields soluble short-chained polymer fragments, facilitating industrial processing and additive removal from chlorinated plastic waste.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 1006-1018"},"PeriodicalIF":0.0,"publicationDate":"2024-06-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00082j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141252726","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
Understanding the charge transfer dynamics in 3D–1D nanocomposites over solar driven synergistic selective valorization of lignocellulosic biomass: a new sustainable approach† 在太阳能驱动的木质纤维素生物质协同选择性增值过程中,了解 3D-1D 纳米复合材料中的电荷转移动力学:一种新的可持续方法
EES catalysis Pub Date : 2024-05-25 DOI: 10.1039/D4EY00077C
Arpna Jaryal, Ajit Kumar Singh, Shivali Dhingra, Himanshu Bhatt, Manvi Sachdeva, Hirendra N. Ghosh, Arindam Indra and Kamalakannan Kailasam
{"title":"Understanding the charge transfer dynamics in 3D–1D nanocomposites over solar driven synergistic selective valorization of lignocellulosic biomass: a new sustainable approach†","authors":"Arpna Jaryal, Ajit Kumar Singh, Shivali Dhingra, Himanshu Bhatt, Manvi Sachdeva, Hirendra N. Ghosh, Arindam Indra and Kamalakannan Kailasam","doi":"10.1039/D4EY00077C","DOIUrl":"10.1039/D4EY00077C","url":null,"abstract":"<p >Photocatalytic redox valorization of lignocellulosic biomass to fine chemicals is in its infancy stages where it can be effectively utilized for sustainable energy conversion. In this direction, an effective 3D–1D (Aeroxide P25 TiO<small><sub>2</sub></small> and CdS) nanocomposite has been demonstrated to upgrade several biomass-derived platform chemicals (<em>e.g.</em> HMF, FFaL, vanillyl alcohol) in a selective and synergistic redox pathway under visible light irradiation for the first time. The successful utilization of the photocatalytic system resulted in the visible light-driven selective hydrogenation of HMF to BHMF along with the coproduction of H<small><sub>2</sub></small> without the addition of any reducing agent under natural sunlight. In addition, the simultaneous production of valuable commodity chemical, <em>i.e.</em> vanillin, through oxidation has also been earmarked. The intimate interfacial contact between CdS as a visible light active photocatalyst and P25 TiO<small><sub>2</sub></small> as an active hydrogenation site assists the facile migration of photogenerated electrons towards P25 TiO<small><sub>2</sub></small>. The coupling of electrons with <em>in situ</em> generated protons led to 95% yield of BHMF whereas oxidative photogenerated holes yielded 35% vanillin, thus abolishing the need for extra redox additives. The synergistic effect bestowed by the semiconductor heterojunction manifested excellent photoredox activity accompanying strong inter-particle interactions which were thoroughly investigated by employing electrochemical, PL, XPS and transient absorption spectroscopy (TAS). Thus, a new sustainable “biomass-based photo-refinery” and cost-effective low carbon-intensity approach has been elucidated for visible light-based hydrogenation activity of TiO<small><sub>2</sub></small> unveiling a fabrication strategy of photocatalysts with efficient solar spectrum harvesting.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 1019-1026"},"PeriodicalIF":0.0,"publicationDate":"2024-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00077c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141147635","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
Sulfur-regulated metal–support interaction boosting the hydrogen evolution performance of Ru clusters in seawater at industrial current densities† 在工业电流密度下,硫调节的金属-支撑相互作用提高了海水中 Ru 簇的氢进化性能
EES catalysis Pub Date : 2024-05-24 DOI: 10.1039/D4EY00076E
Ranran Tang, Ping Yan, Yitong Zhou and Xin-Yao Yu
{"title":"Sulfur-regulated metal–support interaction boosting the hydrogen evolution performance of Ru clusters in seawater at industrial current densities†","authors":"Ranran Tang, Ping Yan, Yitong Zhou and Xin-Yao Yu","doi":"10.1039/D4EY00076E","DOIUrl":"10.1039/D4EY00076E","url":null,"abstract":"<p >Regulating the metal–support interaction (MSI) is an effective strategy to enhance the catalytic activity of electrocatalysts. Herein, taking Ru clusters as an example, we report a hybrid electrocatalyst with ultrafine Ru nanoclusters anchored on sulfur and nitrogen co-doped carbon (Ru/SNC) hollow spheres for efficient hydrogen evolution reaction (HER) in an alkaline electrolyte and real seawater. The optimal Ru/SNC hollow spheres on a glassy carbon electrode exhibit superior HER activity, with small overpotentials of only 12 and 30 mV to reach 10 mA cm<small><sup>−2</sup></small> in alkaline media and alkaline real seawater, respectively. When loaded on carbon paper, the Ru/SNC hollow spheres only need small overpotentials of 171 (in alkaline solution) and 205 mV (in alkaline real seawater) to deliver an industrial current density of 1000 mA cm<small><sup>−2</sup></small>. Furthermore, the assembled Ru/SNC||RuO<small><sub>2</sub></small> electrolysis cell displays a high current density of 1000 mA cm<small><sup>−2</sup></small> at a cell voltage of 2.3 V and impressive stability up to 100 h at a current density of 1000 mA cm<small><sup>−2</sup></small> in alkaline real seawater at an elevated temperature of 80 °C. Density functional theory (DFT) calculations suggest that S-doping can induce a strong MSI between Ru clusters and the carbon support to boost the HER activity and stability. S-doping triggers the downshift of the d-band center, weakening the adsorption of H* on Ru clusters and thereby enhancing the hydrogen spillover.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 932-940"},"PeriodicalIF":0.0,"publicationDate":"2024-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00076e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141147657","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
Operational strategies of pulsed electrolysis to enhance multi-carbon product formation in electrocatalytic CO2 reduction† 在电催化二氧化碳还原过程中加强多碳产物形成的脉冲电解操作策略
EES catalysis Pub Date : 2024-05-16 DOI: 10.1039/D4EY00039K
Takashi Ito, Jithu Raj, Tianyu Zhang, Soumyabrata Roy and Jingjie Wu
{"title":"Operational strategies of pulsed electrolysis to enhance multi-carbon product formation in electrocatalytic CO2 reduction†","authors":"Takashi Ito, Jithu Raj, Tianyu Zhang, Soumyabrata Roy and Jingjie Wu","doi":"10.1039/D4EY00039K","DOIUrl":"10.1039/D4EY00039K","url":null,"abstract":"<p >The electrocatalytic reduction of CO<small><sub>2</sub></small> offers a promising avenue for converting anthropogenic CO<small><sub>2</sub></small> into valuable chemical and fuel feedstocks. Copper (Cu) catalysts have shown potential in this regard, yet challenges persist in achieving high selectivity for multi-carbon (C<small><sub>2+</sub></small>) products. Pulsed electrolysis, employing alternating anodic and cathodic potentials (<em>E</em><small><sub>a</sub></small>/<em>E</em><small><sub>c</sub></small>) or two different cathodic potentials (<em>E</em><small><sub>c1</sub></small>/<em>E</em><small><sub>c2</sub></small>), presents a promising approach to modulate activity and selectivity. In this study, we investigate the influence of catalyst morphology and operational strategies on C<small><sub>2+</sub></small> product formation using Cu nanoparticles (NPs) and CuO nanowires (NWs) in flow cells. In <em>E</em><small><sub>a</sub></small>/<em>E</em><small><sub>c</sub></small> mode, commercial Cu NPs show negligible promotion of C<small><sub>2+</sub></small> selectivity while CuO NWs demonstrate enhanced C<small><sub>2+</sub></small> selectivity attributed to facile oxidation/redox cycling and grain boundary formation. In contrast, <em>E</em><small><sub>c1</sub></small>/<em>E</em><small><sub>c2</sub></small> pulsed electrolysis promotes C<small><sub>2+</sub></small> yield across various catalyst morphologies by enhancing CO<small><sub>2</sub></small> accumulation, pH effect, and supplemental CO utilization. We further extend our investigation to membrane electrode assembly cells, highlighting the potential for scalability and commercialization. Our findings underscore the importance of catalyst morphology and operational strategies in optimizing C<small><sub>2+</sub></small> product formation pulsed electrolysis, laying the groundwork for future advancements in CO<small><sub>2</sub></small> electroreduction technologies.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 997-1005"},"PeriodicalIF":0.0,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00039k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141062748","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
Variable-valence element doping mediated photogenerated electron trapping for selective oxidation reactions† 可变价元素掺杂介导的光生电子捕获用于选择性氧化反应
EES catalysis Pub Date : 2024-04-24 DOI: 10.1039/D4EY00024B
Xia Zhong, Yan Zhao, Lei Li, Xin He, Hui Wang, Xiaodong Zhang and Yi Xie
{"title":"Variable-valence element doping mediated photogenerated electron trapping for selective oxidation reactions†","authors":"Xia Zhong, Yan Zhao, Lei Li, Xin He, Hui Wang, Xiaodong Zhang and Yi Xie","doi":"10.1039/D4EY00024B","DOIUrl":"10.1039/D4EY00024B","url":null,"abstract":"<p >Photocatalytic selective oxidation provides a green and mild way of producing high-value added chemicals, whose conversion and selectivity are limited by complex oxidation pathways mediated by various reactive radical species. Thus, using photogenerated holes as an oxidant to directly drive these oxidation reactions could overcome the above problems, whereas the simultaneously formed electrons would cause the quenching of holes or the formation of other unfavorable reactive oxygen species that would affect the reaction efficiency. Herein, a variable-valence element doping method was proposed to realize hole-mediated photocatalytic selective oxidation. By taking Cu-doped Bi<small><sub>2</sub></small>WO<small><sub>6</sub></small> as a typical prototype, we show that the doped Cu element with monovalent and divalent character can effectively trap photogenerated electrons, thereby boosting hole accumulation for selective oxidation reactions. As expected, Cu-doped Bi<small><sub>2</sub></small>WO<small><sub>6</sub></small> exhibited excellent catalytic performances in oxidative coupling of benzylamines. This study provides a perspective on optimizing selective oxidation by hole regulation.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 980-986"},"PeriodicalIF":0.0,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00024b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140798511","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
Correction: Advanced bifunctional catalyst design for rechargeable zinc–air batteries 更正:用于锌-空气充电电池的先进双功能催化剂设计
EES catalysis Pub Date : 2024-04-23 DOI: 10.1039/D4EY90010C
Tao Wang, Zezhong Shi, Faxing Wang, Jiarui He, Yiren Zhong, Yuan Ma, Zhi Zhu, Xin-Bing Cheng, Kenneth I. Ozoemena and Yuping Wu
{"title":"Correction: Advanced bifunctional catalyst design for rechargeable zinc–air batteries","authors":"Tao Wang, Zezhong Shi, Faxing Wang, Jiarui He, Yiren Zhong, Yuan Ma, Zhi Zhu, Xin-Bing Cheng, Kenneth I. Ozoemena and Yuping Wu","doi":"10.1039/D4EY90010C","DOIUrl":"10.1039/D4EY90010C","url":null,"abstract":"<p >Correction for ‘Advanced bifunctional catalyst design for rechargeable zinc–air batteries’ by Tao Wang <em>et al.</em>, <em>EES. Catal.</em>, 2024, https://doi.org/10.1039/d4ey00014e.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 874-874"},"PeriodicalIF":0.0,"publicationDate":"2024-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey90010c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140798528","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
Structural selectivity of supported Pd nanoparticles: selective ethanol ammoxidation to acetonitrile† 支撑钯纳米粒子的结构选择性:选择性乙醇氨氧化成乙腈
EES catalysis Pub Date : 2024-04-18 DOI: 10.1039/D4EY00044G
Khaled Mohammed, Reza Vakili, Donato Decarolis, Shaojun Xu, Luke Keenan, Apostolos Kordatos, Nikolay Zhelev, Chris K. Skylaris, Marina Carravetta, Emma K. Gibson, Haresh Manyar, Alexandre Goguet and Peter P. Wells
{"title":"Structural selectivity of supported Pd nanoparticles: selective ethanol ammoxidation to acetonitrile†","authors":"Khaled Mohammed, Reza Vakili, Donato Decarolis, Shaojun Xu, Luke Keenan, Apostolos Kordatos, Nikolay Zhelev, Chris K. Skylaris, Marina Carravetta, Emma K. Gibson, Haresh Manyar, Alexandre Goguet and Peter P. Wells","doi":"10.1039/D4EY00044G","DOIUrl":"10.1039/D4EY00044G","url":null,"abstract":"<p >The need to achieve net zero requires decarbonisation across all areas of our industrialised society, including the production of chemicals. One example is the production of acetonitrile, which currently relies on fossil carbon. Recently, supported Pd nanoparticles have been shown to promote the selective transformation of bio-derived ethanol to acetonitrile. Elsewhere, current research has demonstrated the importance of interstitial structures of Pd in promoting specific transformations. In this study, we demonstrate through a spatially resolved <em>operando</em> energy-dispersive-EXAFS (EDE) technique that selectivity to acetonitrile (up to 99%) is concurrent with the formation of a PdN<small><sub><em>x</em></sub></small> phase. This was evidenced from the features observed in the X-ray absorption near edge structure that were validated against PdN<small><sub><em>x</em></sub></small> samples made <em>via</em> known synthesis methods. Above 240 °C, the Pd nanoparticles became progressively oxidised which led to the production of unwanted byproducts, primarily CO<small><sub>2</sub></small>. The spatially resolved analysis indicated that the Pd speciation was homogeneous across the catalyst profile throughout the series of studies performed. This work resolved the structural selectivity of Pd nanoparticles that directs ethanol ammoxidation towards acetonitrile, and provides important information on the performance descriptors required to advance this technology.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 987-996"},"PeriodicalIF":0.0,"publicationDate":"2024-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00044g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140613085","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
Probing the active sites of oxide encapsulated electrocatalysts with controllable oxygen evolution selectivity† 探究具有可控氧进化选择性的氧化物封装电催化剂的活性位点
EES catalysis Pub Date : 2024-04-17 DOI: 10.1039/D4EY00074A
William D. H. Stinson, Robert S. Stinson, Jingjing Jin, Zejie Chen, Mingjie Xu, Fikret Aydin, Yinxian Wang, Marcos F. Calegari Andrade, Xiaoqing Pan, Tuan Anh Pham, Katherine E. Hurst, Tadashi Ogitsu, Shane Ardo and Daniel V. Esposito
{"title":"Probing the active sites of oxide encapsulated electrocatalysts with controllable oxygen evolution selectivity†","authors":"William D. H. Stinson, Robert S. Stinson, Jingjing Jin, Zejie Chen, Mingjie Xu, Fikret Aydin, Yinxian Wang, Marcos F. Calegari Andrade, Xiaoqing Pan, Tuan Anh Pham, Katherine E. Hurst, Tadashi Ogitsu, Shane Ardo and Daniel V. Esposito","doi":"10.1039/D4EY00074A","DOIUrl":"10.1039/D4EY00074A","url":null,"abstract":"<p >Electrocatalysts encapsulated by nanoscopic overlayers can control the rate of redox reactions at the outer surface of the overlayer or at the buried interface between the overlayer and the active catalyst, leading to complex behavior in the presence of two competing electrochemical reactions. This study investigated oxide encapsulated electrocatalysts (OECs) comprised of iridium (Ir) thin films coated with an ultrathin (2–10 nm thick) silicon oxide (SiO<small><sub><em>x</em></sub></small>) or titanium oxide (TiO<small><sub><em>x</em></sub></small>) overlayer. The performance of SiO<small><sub><em>x</em></sub></small>|Ir and TiO<small><sub><em>x</em></sub></small>|Ir thin film electrodes towards the oxygen evolution reaction (OER) and Fe(<small>II</small>)/Fe(<small>III</small>) redox reactions were evaluated. An improvement in selectivity towards the OER was observed for all OECs. Overlayer properties, namely ionic and electronic conductivity, were assessed using a combination of electroanalytical methods and molecular dynamics simulations. SiO<small><sub><em>x</em></sub></small> and TiO<small><sub><em>x</em></sub></small> overlayers were found to be permeable to H<small><sub>2</sub></small>O and O<small><sub>2</sub></small> such that the OER can occur at the MO<small><sub><em>x</em></sub></small>|Ir (M = Ti, Si) buried interface, which was further supported with molecular dynamics simulations of model SiO<small><sub>2</sub></small> coatings. In contrast, Fe(<small>II</small>)/Fe(<small>III</small>) redox reactions occur to the same degree with TiO<small><sub><em>x</em></sub></small> overlayers having thicknesses less than 4 nm as bare electrocatalyst, while SiO<small><sub><em>x</em></sub></small> overlayers inhibit redox reactions at all thicknesses. This observation is attributed to differences in electronic transport between the buried interface and outer overlayer surface, as measured with through-plane conductivity measurements of wetted overlayer materials. These findings reveal the influence of oxide overlayer properties on the activity and selectivity of OECs and suggest opportunities to tune these properties for a wide range of electrochemical reactions.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 953-967"},"PeriodicalIF":0.0,"publicationDate":"2024-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00074a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140582631","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
Epitaxial heterointerfacial electron bridge synchronizes oxygen evolution activity and stability on a layered double hydroxide surface† 层状双氢氧化物表面的外延异表面电子桥同步提高了氧进化活性和稳定性
EES catalysis Pub Date : 2024-04-02 DOI: 10.1039/D4EY00037D
Jia Wang, Zelin Zhao, Min Guo, Liang Xiao, Haolin Tang, Jiantao Li, Zongkui Kou and Junsheng Li
{"title":"Epitaxial heterointerfacial electron bridge synchronizes oxygen evolution activity and stability on a layered double hydroxide surface†","authors":"Jia Wang, Zelin Zhao, Min Guo, Liang Xiao, Haolin Tang, Jiantao Li, Zongkui Kou and Junsheng Li","doi":"10.1039/D4EY00037D","DOIUrl":"10.1039/D4EY00037D","url":null,"abstract":"<p >Scalable green hydrogen production <em>via</em> electrocatalytic water splitting is largely restricted by the insufficient activity and stability of oxygen evolution reaction (OER) catalysts at the anode. As a class of the most active OER catalysts in alkaline electrolyzers, the application of layered double hydroxides (LDHs) remains a main challenge owing to the unstable lattice oxygen dissolution due to the dominant lattice oxygen-involving OER mechanism during long-term operation. Herein, we found that using an epitaxial hetero-interfacing nickel hydroxide (namely Ni(OH)<small><sub>2</sub></small>) as an electron bridge between an active FeCo LDH and Ni foam support to form an LDH*/NFO catalyst, the electronic storage capacity around the Fermi level (−0.5 to +0.5 eV, e-D<small><sub>FE</sub></small>) sharply increases from 0.93 per cell to 1.51 per cell. Subsequently, we demonstrate that this high e-D<small><sub>FE</sub></small> enables ceaseless and fast power injection into the kinetic process of intermediate species conversion and inhibits lattice oxygen dissolution in the active FeCo LDH. Consequently, it demonstrated a low OER overpotential of 246 mV at a current density of 100 mA cm<small><sup>−2</sup></small> and ultrahigh stability for up to 3500 hours with an ultraslow overpotential increase rate of 9.4 × 10<small><sup>−3</sup></small> mV h<small><sup>−1</sup></small>. Therefore, we developed an epitaxial hetero-interfacial electron bridging strategy to synchronize the activity and stability of available catalysts for scalable green hydrogen production <em>via</em> electrocatalytic water splitting.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 862-873"},"PeriodicalIF":0.0,"publicationDate":"2024-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00037d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140582636","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
Zeolite catalysts for non-oxidative ethane dehydrogenation to ethylene 用于非氧化乙烷脱氢制乙烯的沸石催化剂
EES catalysis Pub Date : 2024-03-19 DOI: 10.1039/D4EY00031E
Lu Liu, Liang Wang and Feng-Shou Xiao
{"title":"Zeolite catalysts for non-oxidative ethane dehydrogenation to ethylene","authors":"Lu Liu, Liang Wang and Feng-Shou Xiao","doi":"10.1039/D4EY00031E","DOIUrl":"10.1039/D4EY00031E","url":null,"abstract":"<p >The conversion of ethane to ethylene is crucial for deriving platform chemicals from non-petroleum feedstock. However, it currently relies on steam cracking technology, which involves high temperatures and large reactors. The catalytic dehydrogenation of ethane (EDH) could resolve these issues, but its efficiency is often limited due to thermodynamics, leading to low conversion and coke formation. These challenges make it difficult for catalytic EDH to compete economically with steam cracking. Recent studies show that rational design of catalysts, such as fixing metal nanoclusters within zeolite micropores or isolated metal sites on the zeolite framework, can enhance catalytic performances. These designs lower energy barriers for carbon–hydrogen bond activation, hinder deep dehydrogenation to coke, and provide sinter-resistant metal sites for durability. This review discusses the pivotal role of zeolite structures in catalysis and sums up the principles of catalyst design for efficient non-oxidative EDH. It aims to help in the development of more efficient zeolite catalysts and enhance the viability of catalytic EDH for potential industrialization.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 923-931"},"PeriodicalIF":0.0,"publicationDate":"2024-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d4ey00031e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140170934","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}
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