Sandeep C. Kanade, Sanchayita Mukhopadhyay, Bhojkumar Nayak, Manu Gautam, Bharat B. Kale, Anil B. Gambhire, Musthafa Ottakam Thotiyl
{"title":"Dual Carbide Heterostructure Interface Mimicking Noble Metal-Like Activity for Reversible Dioxygen Catalysis in Rechargeable Air Batteries","authors":"Sandeep C. Kanade, Sanchayita Mukhopadhyay, Bhojkumar Nayak, Manu Gautam, Bharat B. Kale, Anil B. Gambhire, Musthafa Ottakam Thotiyl","doi":"10.1021/acsaem.4c01499","DOIUrl":"https://doi.org/10.1021/acsaem.4c01499","url":null,"abstract":"Recently, there has been significant interest in replacing expensive electrocatalysts with efficient bifunctional materials for facilitating dioxygen redox. Transition-metal carbides, known for their conductivity and mechanical strength, are promising toward this purpose. However, their lower activity and the resulting impact on commercial viability continue to present significant challenges. This study introduces a unique method for creating heterostructured interface comprising molybdenum carbide and vanadium carbide supported on nitrogen-doped graphene (MVC) for catalyzing dioxygen redox chemistry oxygen reduction reactions (ORR) and oxygen evolution reactions (OER) with activity comparable to noble metals. MVC exhibits performance metrics comparable to Pt in the ORR and required only half the overpotential to catalyze the OER at the desired rate compared to its individual counterparts. Improved dioxygen redox is attributed to heterostructure-assisted electron density modulation of the active redox species (required for OER and ORR) in MVC. Integration of MVC into a laboratory-level zinc–air battery prototype demonstrated almost similar round-trip efficiency compared to the benchmark Pt/C + RuO<sub>2</sub> electrocatalyst, indicating its potential as an inexpensive bifunctional electrocatalyst.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Salman, Sumaiya Saleem, Yihan Ling, Majid Khan
{"title":"Fe-Based High-Entropy Perovskite Oxide: A Strategy to Suppress Sr Segregation and Performance Evaluation as an Electrode Material for SOFCs","authors":"Muhammad Salman, Sumaiya Saleem, Yihan Ling, Majid Khan","doi":"10.1021/acsaem.4c01614","DOIUrl":"https://doi.org/10.1021/acsaem.4c01614","url":null,"abstract":"The development of symmetrical solid oxide fuel cells (SSOFCs) has been restricted by the challenge of finding electrode materials that are both highly active and stable. Sr segregation on the surface of perovskite oxides can also significantly affect the durability and oxygen reduction activity of the SSOFC electrodes. In this study, the concept of high-entropy electrodes is proposed, and a high-entropy perovskite oxide La<sub>0.2</sub>Pr<sub>0.2</sub>Eu<sub>0.2</sub>Ce<sub>0.2</sub>Sr<sub>0.2</sub>FeO<sub>3−δ</sub> (HEP-LSF) was fabricated and examined as a favorable electrode material for SSOFCs. The catalytic activity and electrochemical performance were significantly improved by partial substitution of Eu, Pr, and Ce into the A-site, whereas the formation of a disorderly stress field around Sr suppressed Sr-segregation during long-term operation. The HEP-LSF cathode attained a remarkably low polarization resistance of 0.136 Ω·cm<sup>2</sup> in yttria-stabilized zirconia (YSZ) at 800 °C, which is almost half (0.265 Ω·cm<sup>2</sup>) of a conventional La<sub>0.2</sub>Sr<sub>0.8</sub>FeO<sub>3−δ</sub> (LSF) cathode under the same conditions. The YSZ-based SSOFC with HEP-LSF electrodes exhibited a power density of 451 mW/cm<sup>2</sup> at 800 °C. More importantly, the SSOFC with HEP-LSF electrodes exhibited good stability at 700 °C for 100 h. Moreover, the electrical conductivity and activation energy for HEP-LSF is higher than LSF which is 18.67 kJ·mol<sup>–1</sup>, and 599.57 S·cm<sup>–1</sup> at 800 °C. These results demonstrate that HEP-LSF suppresses Sr segregation and has outstanding potential as an electrode material for SSOFC, thus making it a promising candidate for practical applications.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Advancing High-Energy Solid-State Batteries with High-Entropy NASICON-type Solid Electrolytes","authors":"Asish Kumar Das, Pratiksha Gami, Hari Narayanan Vasavan, Samriddhi Saxena, Neha Dagar, Sonia Deswal, Pradeep Kumar, Sunil Kumar","doi":"10.1021/acsaem.4c02011","DOIUrl":"https://doi.org/10.1021/acsaem.4c02011","url":null,"abstract":"Herein, we have developed a <i>High-Entropy</i> (<i>∼1.52 R</i>, calculated at M-site) lithium-stuffed NASICON-type solid electrolyte [Li<sub>1.3</sub>Sn<sub>1.7/3</sub>Zr<sub>1.7/3</sub>Ti<sub>1.7/3</sub>Al<sub>0.1</sub>Sc<sub>0.1</sub>Y<sub>0.1</sub>(PO<sub>4</sub>)<sub>3</sub>] with a total (grain + grain-boundary) ionic conductivity of ∼1.42 × 10<sup>–4</sup> S cm<sup>–1</sup> (highest reported among NASICONs containing Zr–Sn–Ti) and a low activation energy of ∼0.33 eV with a relative density of <i>Conventionally Sintered</i> pellet ∼94%. Symmetric cells with a PVDF-HFP/LiTFSI buffer layer showed stable performance for 500 cycles at 0.2 mA cm<sup>–2</sup> without short-circuiting. Full cells with LiFePO<sub>4</sub> retained ∼99% capacity after 100 cycles at 1C, while those with NMC811 delivered ∼140 mAh g<sup>–1</sup> at C/3.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Tunable Production of Syngas via Pulsed-Potential Electrolysis of CO2 over Single-Crystal Cu(100)","authors":"Yue Gong, Tao He","doi":"10.1021/acsaem.4c01338","DOIUrl":"https://doi.org/10.1021/acsaem.4c01338","url":null,"abstract":"Obtaining syngas from the electrochemical reduction of CO<sub>2</sub> has been considered an economical and promising solution for energy and environmental sustainability. Cu-based catalysts have been attracting great attention due to their low cost and easy accessibility, while tuning the selectivity toward specific products is a critical issue. In this work, a pulsed-potential strategy coupled with a low-reduction overpotential is applied to (100) single-crystal Cu foils. Only H<sub>2</sub> and CO are observed under the bias of a low-reduction potential. By tuning the pulse width and anodic potential, controllable syngas with a broad range from ∼97:5 to ∼5:14 can be obtained with the same low cathodic potential. Based on various characterization results before and after pulse electrolysis, the enhanced CO production is attributed to the in situ-generated Cu<sup>+</sup> species and roughened surface, as well as the modulation of local pH and CO<sub>2</sub> concentration near the electrode.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264301","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Angela G. Selva Ochoa, Faezeh Habibzadeh, Elod L. Gyenge
{"title":"Robust Bi Metal–Organic Framework-Derived Catalyst for the Selective Electroreduction of CO2 to Formate at Current Densities up to 1 A cm–2 in Gas Diffusion Electrodes","authors":"Angela G. Selva Ochoa, Faezeh Habibzadeh, Elod L. Gyenge","doi":"10.1021/acsaem.4c01845","DOIUrl":"https://doi.org/10.1021/acsaem.4c01845","url":null,"abstract":"Electrochemical reduction of CO<sub>2</sub> to useful products requires selective and stable catalysts that can be easily synthesized and are cost-effective. In this work, we investigate the Bi CAU-17 metal–organic framework (MOF) synthesized by a novel and scalable method to generate in situ highly active Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> catalyst for CO<sub>2</sub> electroreduction to formate in either KHCO<sub>3</sub> or KOH electrolytes. The Bi CAU-17-derived catalyst provides high faradaic efficiencies toward formate (FE<sub>HCOO</sub><sup>–</sup> = 85–100%) at current densities up to 1 A cm<sup>–2</sup> in a gas diffusion electrode with a low catalyst loading (0.5 mg cm<sup>–2</sup>). Comparative experiments between commercial and in situ generated Bi<sub>2</sub>O<sub>2</sub>CO<sub>3</sub> from Bi CAU-17 showed that the latter has superior catalytic performance at high current densities (>300 mA cm<sup>–2</sup>) and with stable activity after 26 h of continuous electrolysis at 200 mA cm<sup>–2</sup> in the pH range 8–14. These results highlight the importance of generating in situ active Bi/Bi–O sites that promote the selective reduction of CO<sub>2</sub> to formate.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
George Perrakis, George Kakavelakis, Anna C. Tasolamprou, Essa A. Alharbi, Konstantinos Petridis, George Kenanakis, Maria Kafesaki
{"title":"Plasmonic Nanoparticles’ Impact on Perovskite–Perovskite Tandem Solar Cells’ Thickness and Weight","authors":"George Perrakis, George Kakavelakis, Anna C. Tasolamprou, Essa A. Alharbi, Konstantinos Petridis, George Kenanakis, Maria Kafesaki","doi":"10.1021/acsaem.4c01991","DOIUrl":"https://doi.org/10.1021/acsaem.4c01991","url":null,"abstract":"In this work, we report on the plasmonic impact of metal nanoparticles of different compositions, sizes, vertical positions, concentrations, and shell thicknesses dispersed inside the mixed (lead–tin) narrow-band gap (NBG) perovskite layer of perovskite–perovskite tandem solar cells (TPSCs) on TPSCs’ (i) NBG thickness reduction, (ii) absorption, and (iii) power-per-weight output (PPW) enhancement. The aim is to establish guidelines for the highly promising development of efficient, viable, and environmentally friendly plasmonic-enhanced tandem solar cells and examine metal nanoparticles’ plasmonic and weight impact on the PPW output of solar cells and tandem configurations by means of a detailed numerical analysis and optimization procedure on TPSC architectures. Based on the high NBG thickness reductions predicted (>650 nm, >60% decrease) and PPW increase (+14 W/g, ∼50% improvement) under current matching conditions with the front wide-band gap subcell, results indicate that enhanced light-trapping (due to localized surface-plasmon effects) combined with metal nanoparticles simplicity at processing provide a means to attain efficient and viable TPSCs using NBG films much thinner than those usually employed (>1 μm), thus facilitating collection of photocarriers, reducing cost and the amount of potentially toxic lead–tin present in the device, and enhancing PPW output. The detailed theoretical analysis serves as a guide for various applications that can benefit from the plasmonic effect and band gap tunability, including photovoltaics of different materials (e.g., perovskite-organic tandems), PPW applications, light-emitting diodes, and sensors, also further promoting the viability of TPSCs in emerging applications such as space applications, portable/wearable electronics, automobiles, or other applications where there is a stringent limitation on the PPW ratio of the photovoltaic panel.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264304","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Regulating the Electrochemical Performance of A2Ni2TeO6 (A = Na, K) as a Cathode of Alkali Metal Ion Battery by 3d Transition Metal Substitution from a Theoretical Perspective","authors":"Zhi-Hai Wu, Yang-Xin Yu","doi":"10.1021/acsaem.4c01667","DOIUrl":"https://doi.org/10.1021/acsaem.4c01667","url":null,"abstract":"With its unique honeycomb layered structure, P2-type A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K) exhibits remarkable cycling stability and ionic diffusion capability, making it a promising cathode material for sodium-ion batteries (SIBs) and potassium-ion batteries (PIBs). However, the high operating voltage of A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K) leading to surface degradation and CEI formation limits the capacity of A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K), where only 2/3 of Na<sup>+</sup> and 1/2 K<sup>+</sup> can be reversibly extracted at a high charge rate. To enhance the capacity of A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K) while maintaining its cycling stability, we delved into the impacts of 3d transition metal substitution on sodium and potassium storage chemistry through first-principles calculations. Our investigation includes multiple facets: lattice structure, substituting formation energy, electronic properties, ionic diffusion, average open-circuit voltage, transition metal migration, and intermediate phases in the high-voltage region. After comprehensive consideration, Mn- and Fe-substituted Na<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> and Fe-substituted K<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> emerged as the most promising candidates, exhibiting exceptional electrochemical performance. Furthermore, we discovered that the energy difference between alkali metal ions occupying substitution sites and active transition metal sites dominates the ionic diffusion behavior in TM-substituted A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K), and the nonuniform distribution of alkali metal ions significantly contributes to the large volume change during ionic extraction. The findings of this work not only underscore the intricate structure–activity relationship of P2-type A<sub>2</sub>Ni<sub>2</sub>TeO<sub>6</sub> (A = Na, K) substitution but also provide theoretical insights for future application of honeycomb layered transition metal oxides (HLOs) in SIB and PIB cathodes.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264303","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bhuvaneshwari Ezhilmaran, Cheol Hyoun Ahn, Won Seok Yang, Hyung Koun Cho
{"title":"Rational Design of a Co/MnO-Embedded 2D Nitrogen-Doped Carbon/Carbon Nanotube Hybrid Catalyst for Efficient Oxygen Catalysis and High-Capacity Zn–Air Batteries","authors":"Bhuvaneshwari Ezhilmaran, Cheol Hyoun Ahn, Won Seok Yang, Hyung Koun Cho","doi":"10.1021/acsaem.4c01412","DOIUrl":"https://doi.org/10.1021/acsaem.4c01412","url":null,"abstract":"Bimetallic catalysts used as air cathodes for Zn–air batteries offer improved activity and performance by tuning the electronic structure and interactions between metals. In particular, the fabrication of metal/metal compound heterostructure-embedded carbon catalysts is required owing to their desired properties; however, this often requires multistep-involved/complex synthesis conditions, hampering large-scale production. In this study, a Co/MnO-embedded nitrogen-doped carbon/carbon nanotube (CM-N:C) was developed by using a simple synthetic strategy that involved heat-treating the intermediate platform of a Co-based two-dimensional zeolitic imidazolate framework (2D ZIF). The 2D leaf-like products from the ZIF led to the exposure of abundant active sites, and the unique carbon/carbon nanotube hybrid structure resulted in the good durability of the developed catalysts. Moreover, owing to the heterojunction interface, modulated electronic configuration, and favorable porous features, the designed catalyst (CM-N:C) exhibited superior oxygen evolution and oxygen reduction catalytic activities. Furthermore, Zn–air batteries loading these catalysts demonstrated excellent performance, with an especially high specific capacity of 841.26 mAh/g<sub>zn</sub> and energy efficiency of 58.8% at 5 mA/cm<sup>2</sup>. This study provides a perspective for the development of efficient electrocatalysts and air cathode materials for sustainable energy conservation systems.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264307","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Manjunatha Kempasiddaiah, Rajib Samanta, Ravi Kumar Trivedi, Dev Shrivastava, Brahmananda Chakraborty, Sudip Barman
{"title":"Single-Crystalline α-Bi2O3 Induced by Nitrogen Doping for Enhanced and Selective CO2 Electroreduction to Formate over a Wide Negative Potential Window","authors":"Manjunatha Kempasiddaiah, Rajib Samanta, Ravi Kumar Trivedi, Dev Shrivastava, Brahmananda Chakraborty, Sudip Barman","doi":"10.1021/acsaem.4c01358","DOIUrl":"https://doi.org/10.1021/acsaem.4c01358","url":null,"abstract":"An efficient method for reducing atmospheric CO<sub>2</sub> involves employing electrochemical CO<sub>2</sub> reduction reactions (ECO<sub>2</sub>RR). Within this context, the ECO<sub>2</sub>RR to formate is recognized as a highly promising pathway to produce value-added fuels and chemicals. However, the challenge lies in suppressing the evolution of CO and H<sub>2</sub> during the electroconversion of CO<sub>2</sub>. In this regard, Bi-MOFs and their derivatives, such as N-doped carbon-supported α-Bi<sub>2</sub>O<sub>3</sub>–CN<sub><i>x</i></sub> and Bi NPs/NC, were examined as potential electrocatalysts for ECO<sub>2</sub>RR. In an aqueous bicarbonate electrolytic solution, the α-Bi<sub>2</sub>O<sub>3</sub>–CN<sub><i>x</i></sub>-600 composites demonstrated a remarkable Faradaic efficiency of 93.8% at −0.79 V vs RHE, with minimal H<sub>2</sub> production. This efficiency was consistently maintained at an average of 91.2% over the wide potential range of −0.69 to −0.99 V vs RHE. Furthermore, high partial current densities were also achieved for α-Bi<sub>2</sub>O<sub>3</sub>–CN<sub><i>x</i></sub>-600 composites in 0.5 M KHCO<sub>3</sub> (−42.59 mA cm<sup>–2</sup> at −0.99 V), displaying excellent durability for over 10 h. The improved catalytic performance and selectivity were ascribed to a higher Bi loading as well as well-dispersed α-Bi<sub>2</sub>O<sub>3</sub> within the carbon frameworks (CN<sub><i>x</i></sub>), providing abundant active sites. Moreover, a higher content of N-doping in the α-Bi<sub>2</sub>O<sub>3</sub>–CN<sub><i>x</i></sub>-600 lattice likely facilitated *OCHO generation. Density functional theory calculations were also utilized to scrutinize the reaction mechanism underlying the CO<sub>2</sub> reduction reaction to formic acid (HCOOH) over α-Bi<sub>2</sub>O<sub>3</sub>(−120) monoclinic and Bi(012) rhombohedral composites. The computed Gibbs free energy changes associated with the reduction of CO<sub>2</sub> to HCOOH and hydrogen (H<sub>2</sub>) formation on the α-Bi<sub>2</sub>O<sub>3</sub> catalyst suggest a potential suppression of the hydrogen evolution reaction (HER), aligning with experimental findings. Hence, these findings suggest that the prepared α-Bi<sub>2</sub>O<sub>3</sub>–CN<sub><i>x</i></sub>-600 catalysts hold significant potential for the efficient electrochemical reduction of CO<sub>2</sub> to fuels.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264306","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Modified Galvanic Cell Synthesis of Pd@Pt Core–Shell Nanowire Catalysts: Structural Insights and Enhanced ORR Performance","authors":"Weijie Cao, Mukesh Kumar, Neha Thakur, Tomoki Uchiyama, Yunfei Gao, Satoshi Tominaka, Akihiko Machida, Toshiki Watanabe, Ryota Sato, Toshiharu Teranishi, Masashi Matsumoto, Hideto Imai, Yoshiharu Sakurai, Yoshiharu Uchimoto","doi":"10.1021/acsaem.4c01444","DOIUrl":"https://doi.org/10.1021/acsaem.4c01444","url":null,"abstract":"One-dimensional nanostructures, specifically Pd@Pt core–shell nanowire catalysts, have garnered significant attention because of their potential to enhance the sluggish kinetics of the oxygen reduction reaction (ORR). However, fully realizing their potential depends on achieving consistent and uniform synthesis. In this study, we introduce an improved galvanic synthesis method for Pd@Pt core–shell nanowire catalysts (Pd-NW@Pt/C) that eliminates the need for electrochemical control or reducing agents, making it more accessible and efficient than the traditional Cu underpotential deposition (Cu-UPD) method. Our approach ensures a uniform Pt shell, resulting in superior ORR activity, with a mass activity of 1.06 A mg<sub>Pt</sub><sup>–1</sup> and a specific activity of 0.80 mA cm<sub>Pt</sub><sup>–2</sup>. Detailed <i>operando</i> X-ray absorption spectroscopy (XAS) measurements, including high-energy resolution fluorescence detection (HERFD-XAS), revealed that Pd-NW@Pt/C catalysts with a fully covered Pt shell exhibit shorter Pt–Pt bond lengths and weaker oxygen binding energies compared to partially covered Pt shell nanowire catalysts (Pd-NW@Pt/C-ref) and nanoparticle catalysts (Pd-NP@Pt/C), leading to significantly enhanced ORR activity. This study demonstrates the effectiveness of a modified galvanic cell method for producing high-performance Pd@Pt core–shell nanowire catalysts, offering insights into their structural and electronic properties.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":6.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142264308","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}