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
Developing promising solid-state Li batteries with capabilities of high current densities have been a major challenge partly due to large interfacial resistance across the electrode/electrolyte interfaces.This work re...Developing promising solid-state Li batteries with capabilities of high current densities have been a major challenge partly due to large interfacial resistance across the electrode/electrolyte interfaces.This work represents an integrated network of self-standing polymer electrolyte and active electrode materials with in situ UV cross-linking.This method provides a uniform morphology of composite polymer electrolyte with low thickness of 20-40μm.This modification leads to promising cycling results with 85%specific capacity retention in LijjLiFePO4 cell over 100 cycles at high current densities of 170 mA g1(~25μA cm^(-2),1 C).By applying this method,the interfacial resistance decreases as high as seven folds compared to noncross-linked interfaces.The following work introduce a facile and cost-effective method in developing fastcharging self-standing polymer batteries with enhanced electrochemical properties.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 science foundation,Grant/Award Number:CBET-1805938Northwestern UniversityUniversity of Illinois at Chicago。
文摘Developing promising solid-state Li batteries with capabilities of high current densities have been a major challenge partly due to large interfacial resistance across the electrode/electrolyte interfaces.This work represents an integrated network of self-standing polymer electrolyte and active electrode materials with in situ UV cross-linking.This method provides a uniform morphology of composite polymer electrolyte with low thickness of 20-40μm.This modification leads to promising cycling results with 85%specific capacity retention in LijjLiFePO4 cell over 100 cycles at high current densities of 170 mA g1(~25μA cm^(-2),1 C).By applying this method,the interfacial resistance decreases as high as seven folds compared to noncross-linked interfaces.The following work introduce a facile and cost-effective method in developing fastcharging self-standing polymer batteries with enhanced electrochemical properties.
