Heteroatom-doped carbon materials have been widely used as sodium(Na) and potassium(K) metal anode frameworks to achieve uniform Na and K depositions. If the origin of the Sodiophilicity and potassiophilicity of dopin...Heteroatom-doped carbon materials have been widely used as sodium(Na) and potassium(K) metal anode frameworks to achieve uniform Na and K depositions. If the origin of the Sodiophilicity and potassiophilicity of doping sites in heteroatom-doped carbon host are clearly understood, the nucleation and growth behavior of Na and K can be precisely regulated in working batteries. Herein the Sodiophilicity and potassiophilicity chemistries of carbon materials are probed through first-principles calculations. The local dipole of doping functional groups and charge transfer during Na/K deposition are regarded as key principles to reveal the sodiophilic and potassiophilic nature of doping sites. Especially, O–B, O–S, and O–P co-doping strategy are predicted to be effective methods to improve the Sodiophilicity and potassiophilicity of carbon hosts and thus render safe and dendrite-free Na and K metal anodes. This work affords a deep and insightful understanding of Sodiophilicity and potassiophilicity chemistry of Na and K anodes and establishes general principles of designing highly sodiophilic and potassiophilic carbon frameworks.展开更多
Potassium metal is regarded as a promising anode material for potassium-ion batteries due to its high theoretical capacity and low redox potential.However,its performance is hindered by rapid capacity fading,primarily...Potassium metal is regarded as a promising anode material for potassium-ion batteries due to its high theoretical capacity and low redox potential.However,its performance is hindered by rapid capacity fading,primarily caused by an unstable solid electrolyte interphase(SEI)and continuous dendrite growth.Herein,by coating liquid metal(LM)alloy(GaInSn)onto copper foil,we prepared a special LM@Cu substrate,significantly improving the deposition/stripping behavior of potassium metal and thus achieving long-cycling K metal battery.The excellent potassiophilicity and electrolyte wettability of LM@Cu effectively reduce the K nucleation overpotential,promote charge transfer kinetics,and enable self-diffusive planar growth mode.Moreover,ex situ scanning electron microscopy and in situ optical microscopy analyses show that the LM coating induces uniform potassium deposition,reduces volume expansion,and achieves a dendrite-free K anode.Additionally,when 3,4,9,10-perylene-tetracarboxylic diimide(PTCDI)is employed as the cathode and K-LM@Cu(LMK)as the anode,the potassium metal battery demonstrates an initial reversible capacity of 124.4 mAh·g^(-1).Even after 4900 cycles at a current density of 500 mA·g^(-1),it maintains a high reversible capacity of 78.2 mAh·g^(-1).The self-diffusive planar growth mechanism enabled by liquid metal offers a promising approach for developing practical and durable potassium metal batteries.展开更多
基金supported by the National Key Research and Development Program(2016YFA0202500)the National Natural Science Foundation of China(21825501)the Tsinghua University Initiative Scientific Research Program。
文摘Heteroatom-doped carbon materials have been widely used as sodium(Na) and potassium(K) metal anode frameworks to achieve uniform Na and K depositions. If the origin of the Sodiophilicity and potassiophilicity of doping sites in heteroatom-doped carbon host are clearly understood, the nucleation and growth behavior of Na and K can be precisely regulated in working batteries. Herein the Sodiophilicity and potassiophilicity chemistries of carbon materials are probed through first-principles calculations. The local dipole of doping functional groups and charge transfer during Na/K deposition are regarded as key principles to reveal the sodiophilic and potassiophilic nature of doping sites. Especially, O–B, O–S, and O–P co-doping strategy are predicted to be effective methods to improve the Sodiophilicity and potassiophilicity of carbon hosts and thus render safe and dendrite-free Na and K metal anodes. This work affords a deep and insightful understanding of Sodiophilicity and potassiophilicity chemistry of Na and K anodes and establishes general principles of designing highly sodiophilic and potassiophilic carbon frameworks.
基金support from the following sources:the National Natural Science Foundation of China(NSFC)(Nos.52171206 and 52271209)the Key Project of Hebei Natural Science Foundation(Nos.F2024201031 and E2020201030)+1 种基金the Science Research Project of Hebei Education Department(No.JCZX2025019)the Interdisciplinary Research Program of Hebei University(No.DXK202401).
文摘Potassium metal is regarded as a promising anode material for potassium-ion batteries due to its high theoretical capacity and low redox potential.However,its performance is hindered by rapid capacity fading,primarily caused by an unstable solid electrolyte interphase(SEI)and continuous dendrite growth.Herein,by coating liquid metal(LM)alloy(GaInSn)onto copper foil,we prepared a special LM@Cu substrate,significantly improving the deposition/stripping behavior of potassium metal and thus achieving long-cycling K metal battery.The excellent potassiophilicity and electrolyte wettability of LM@Cu effectively reduce the K nucleation overpotential,promote charge transfer kinetics,and enable self-diffusive planar growth mode.Moreover,ex situ scanning electron microscopy and in situ optical microscopy analyses show that the LM coating induces uniform potassium deposition,reduces volume expansion,and achieves a dendrite-free K anode.Additionally,when 3,4,9,10-perylene-tetracarboxylic diimide(PTCDI)is employed as the cathode and K-LM@Cu(LMK)as the anode,the potassium metal battery demonstrates an initial reversible capacity of 124.4 mAh·g^(-1).Even after 4900 cycles at a current density of 500 mA·g^(-1),it maintains a high reversible capacity of 78.2 mAh·g^(-1).The self-diffusive planar growth mechanism enabled by liquid metal offers a promising approach for developing practical and durable potassium metal batteries.
