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 ac...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 pyrolysis.Ab initio molecular dynamics(AIMD)calculations are employed to gain a more profound understanding of the impact of acid activation on carbon paper.Furthermore,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 performance.Notably,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 electrodes.The self-standing electrode,featuring harmoniously coexisting Ru states,stands out as a prospective choice for advancing HER catalysts,enhancing energy efficiency,productivity,and selectivity.展开更多
Monitoring taste-inducing ions and molecules continuously in liquids or solutions is of great considerable matter for the realization of the electronic tongue(E-tongue).Particularly from the five major tastes,the high...Monitoring taste-inducing ions and molecules continuously in liquids or solutions is of great considerable matter for the realization of the electronic tongue(E-tongue).Particularly from the five major tastes,the highly selective,sensitive detection of Na^(+)in real-time is prioritized.Prioritization is due to the saltiness of food is the key ingredient in most meals.Nevertheless,existing Na^(+)detecting devices have relatively low performances of selectivity,sensitivity,and lack of on–off functions.Additionally,conventional devices significantly deteriorate in capac-ity due to repetitive usage or lifetime shortage by degradation of the sensing mate-rial.Herein,a graphene-based channel was rationally designed by the facile decoration of Calix[4]arene and Nafion to address this issue.They act as a receptor and a molecular sieve,respectively,to enhance selectivity and sensitivity and elon-gate the life expectancy of the device.This device was merged with a microfluidic channel to control the injection and withdrawal of solutions to fulfill dynamic on–off functions.The fabricated device has highly selective,sensitive Na^(+)detection properties compared to other 10 molecule/ionic species.Dynamic on–off functions of the device were available,also possesses a long lifespan of at least 220 days.Additionally,it can precisely discriminate real beverages containing Na^(+),which can be observed by principal component analysis plot.These features offer the possibility of ascending to a platform for E-tongues in near future.展开更多
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 a...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 activity.Among SACs,metal–organic frameworks(MOFs)have been recognized as promising support materials because of their exceptional ability to prevent metal aggregation.This 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 potential.These 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 pyrolysis.Furthermore,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.展开更多
基金supported by the National Research Foundation of Korea(NRF),funded by the Korean government(2022M3H4A1A01012712,2022M3H4A1A04096380)S.Back acknowledges the support from the National Research Foundation of Korea(NRF)funded by the Ministry of Education(NRF-2016R1A6A1A03012845)and generous supercomputing time from KISTI.
文摘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 pyrolysis.Ab initio molecular dynamics(AIMD)calculations are employed to gain a more profound understanding of the impact of acid activation on carbon paper.Furthermore,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 performance.Notably,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 electrodes.The self-standing electrode,featuring harmoniously coexisting Ru states,stands out as a prospective choice for advancing HER catalysts,enhancing energy efficiency,productivity,and selectivity.
基金National R&D Program,Grant/Award Number:2021M3H4A3A02086430Nano Material Technology Development Program,Grant/Award Number:2022M3H4A1A01011993+3 种基金Ministry of Science and ICT,South KoreaResearch Institute of Advanced Materials(RIAM)Inter University Semiconductor Research Center(ISRC)National Instrumentation Center for Environmental Management(NICEM)。
文摘Monitoring taste-inducing ions and molecules continuously in liquids or solutions is of great considerable matter for the realization of the electronic tongue(E-tongue).Particularly from the five major tastes,the highly selective,sensitive detection of Na^(+)in real-time is prioritized.Prioritization is due to the saltiness of food is the key ingredient in most meals.Nevertheless,existing Na^(+)detecting devices have relatively low performances of selectivity,sensitivity,and lack of on–off functions.Additionally,conventional devices significantly deteriorate in capac-ity due to repetitive usage or lifetime shortage by degradation of the sensing mate-rial.Herein,a graphene-based channel was rationally designed by the facile decoration of Calix[4]arene and Nafion to address this issue.They act as a receptor and a molecular sieve,respectively,to enhance selectivity and sensitivity and elon-gate the life expectancy of the device.This device was merged with a microfluidic channel to control the injection and withdrawal of solutions to fulfill dynamic on–off functions.The fabricated device has highly selective,sensitive Na^(+)detection properties compared to other 10 molecule/ionic species.Dynamic on–off functions of the device were available,also possesses a long lifespan of at least 220 days.Additionally,it can precisely discriminate real beverages containing Na^(+),which can be observed by principal component analysis plot.These features offer the possibility of ascending to a platform for E-tongues in near future.
基金National Research Foundation of Korea(NRF),Grant/Award Numbers:2021R1A4A3027878,RS‐2023‐00209139,2015M3D3A1A01064929Korea Institute of Energy Technology&Energy(MOTIE)of the Republic of Korea,Grant/Award Number:20212010100040。
文摘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 activity.Among SACs,metal–organic frameworks(MOFs)have been recognized as promising support materials because of their exceptional ability to prevent metal aggregation.This 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 potential.These 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 pyrolysis.Furthermore,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.