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Crystallographically vacancy‐induced MOF nanosheet as rational single‐atom support for accelerating CO_(2)electroreduction to CO

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Carbon Energy 2024年第8期6卷 49-62页

作者： Jin Hyuk Cho Joonhee Ma Chaehyeon lee Jin Wook Lim Youngho Kim Ho Yeon Jang Jaehyun Kim Myung‐gi Seo Youngheon Choi Youn Jeong Jang Sang Hyun Ahn Ho Won Jang seoin back.jong‐lam lee Soo Young Kim Department of Materials Science and Engineering Korea UniversitySeoulRepublic of Korea Department of Chemical and Biomolecular Engineering Sogang UniversitySeoulRepublic of Korea Department of Materials Science and Engineering Pohang University of Science and Technology(POSTECH)PohangRepublic of Korea Department of Materials Science and Engineering Research Institute of Advanced MaterialsSeoul National UniversitySeoulRepublic of Korea Lotte Chemical R&D Center DaejeonRepublic of Korea Department of Chemical Engineering Hanyang UniversitySeoulRepublic of Korea School of Chemical Engineering and Material Science Chung‐Ang UniversitySeoulRepublic of Korea

To attain a circular carbon economy and resolve CO_(2)electroreduction technology obstacles,single‐atom catalysts(SACs)have emerged as a logical option for electrocatalysis because of their extraordinary catalytic *** SACs,metal–organic frameworks(MOFs)have been recognized as promising support materials because of their exceptional ability to prevent metal *** study shows that atomically dispersed Ni single atoms on a precisely engineered MOF nanosheet display a high Faradaic efficiency of approximately 100%for CO formation in H‐cell and three‐compartment microfluidic flow‐cell reactors and an excellent turnover frequency of 23,699 h−1,validating their intrinsic catalytic *** results suggest that crystallographic variations affect the abundant vacancy sites on the MOF nanosheets,which are linked to the evaporation of Zn‐containing organic linkers during ***,using X‐ray absorption spectroscopy and density functional theory calculations,a comprehensive investigation of the unsaturated atomic coordination environments and the underlying mechanism involving CO^(*)preadsorbed sites as initial states was possible and provided valuable insights.

关键词： 2‐dimensional material carbon dioxide reduction metal-organic frameworks single‐atom catalysts vacancy sites

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Unraveling the Harmonious Coexistence of Ruthenium States on a Self-Standing Electrode for Enhanced Hydrogen Evolution Reaction

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Energy & Environmental Materials 2024年第6期7卷 303-311页

作者： Joonhee Ma Jin Hyuk Cho Chaehyeon lee Moon Sung Kang Sungkyun Choi Ho Won Jang Sang Hyun Ahn seoin back Soo Young Kim Department of Materials Science and Engineering Korea UniversitySeoul 02841Korea Department of Chemical and Biomolecular Engineering Institute of Emergent MaterialsSogang UniversitySeoul 04107Korea Department of Cogno-Mechatronics Engineering College of Nanoscience and NanotechnologyPusan National UniversityBusan 46241Korea Department of Materials Science and Engineering Research Institute of Advanced MaterialsSeoul National UniversitySeoul 08826Korea School of Chemical Engineering and Material Science Chung-Ang UniversitySeoul 06974Korea

The development of cost-effective,highly efficient,and durable electrocatalysts has been a paramount pursuit for advancing the hydrogen evolution reaction(HER).Herein,a simplified synthesis protocol was designed to achieve a self-standing electrode,composed of activated carbon paper embedded with Ru single-atom catalysts and Ru nanoclusters(ACP/Ru_(SAC+C))via acid activation,immersion,and high-temperature *** initio molecular dynamics(AIMD)calculations are employed to gain a more profound understanding of the impact of acid activation on carbon ***,the coexistence states of the Ru atoms are confirmed via aberration-corrected scanning transmission electron microscopy(AC-STEM),X-ray photoelectron spectroscopy(XPS),and X-ray absorption spectroscopy(XAS).Experimental measurements and theoretical calculations reveal that introducing a Ru single-atom site adjacent to the Ru nanoclusters induces a synergistic effect,tuning the electronic structure and thereby significantly enhancing their catalytic ***,the ACP/Ru_(SAC+C)exhibits a remarkable turnover frequency(TOF)of 18 s^(−1)and an exceptional mass activity(MA)of 2.2 A mg^(−1),surpassing the performance of conventional Pt *** self-standing electrode,featuring harmoniously coexisting Ru states,stands out as a prospective choice for advancing HER catalysts,enhancing energy efficiency,productivity,and selectivity.

关键词： electrocatalysis electronic coupling effect hydrogen evolution reaction selfstanding electrode

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Upcycling end of lithium cobalt oxide batteries to electrocatalyst for oxygen reduction reaction in direct methanol fuel cell via sustainable approach

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Journal of Energy Chemistry 2023年第7期82卷 148-157,I0004页

作者： Keyru Serbara Bejigo Kousik Bhunia Jungho Kim Chaehyeon lee seoin back Sang-Jae Kim Nanomaterials&System Lab Major of Mechatronics EngineeringFaculty of Applied Energy SystemJeju National UniversityJeju 63243Republic of Korea Nanomaterials&System Lab Major of Mechanical System EngineeringCollege of EngineeringJeju National UniversityJeju 63243Republic of Korea Research Institute of New Energy Industry(RINEI) Jeju National UniversityJeju 63243Republic of Korea Department of Chemical and Biomolecular Engineering Institute of Emergent MaterialsSogang UniversitySeoul 04107Republic of Korea

Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable *** typical SLIBs recycling concentrated on separating valuable components had limitations,including high energy consumption and complicated separation *** work suggests a safe hydrometallurgical process to recover usable metallic cobalt from depleted LiCoO_(2)batteries by utilizing citric acid as leachant and hydrogen peroxide as an oxidizing agent,with ethanol as a selective precipitating *** anode graphite was also recovered and converted to graphene oxide(GO).The above components were directly resynthesized to cobaltintegrated nitrogen-doped graphene(Co@NG).The Co@NG showed a decent activity towards oxygen reduction reaction(ORR)with a half-wave potential of 0.880 V ***,almost similar to Pt/C(0.888 V ***)and with an onset potential of 0.92 V *** metal-nitrogen-carbon(Co-N-C)having the highest nitrogen content has decreased the barrier for ORR since the reaction was enhanced for Co@NG-800,as confirmed by density functional theory(DFT)*** Co@NG cathode catalyst coupled with commercial Pt-Ru/C as anode catalyst exhibits excellent performance for direct methanol fuel cell(DMFC)with a peak power density of 34.7 mW cm^(-2)at a discharge current density of120 m A cm^(-2)and decent stability,indicating the promising utilization of spent battery materials in DMFC ***,lithium was recovered from supernatant as lithium carbonate by coprecipitation *** work avoids sophisticated elemental separation by utilizing SLIBs for other renewable energy applications,lowering the environmental concerns associated with recycling.

关键词： Density functional theory(DFT) Direct methanol fuel cell Leaching Nitrogen doping Oxygen reduction reaction Recycling Spent lithium-ion batteries

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