Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen...Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen evolution reaction(OER)due to their layered structure combined with versatile com-positions.Furthermore,reducing the thickness of platelet LDH crystals to nanometer or even molecular scale via cleavage or delamination provides an important clue to enhance the activity.In this review,recent progresses on rational design of LDH nanosheets are reviewed,including direct synthesis via traditional coprecipitation,homogeneous precipitation,and newly developed topochemical oxidation as well as chemical exfoliation of parent LDH crystals.In addition,diverse strategies are introduced to modulate their electrochemical activity by tuning the composition of host metal cations and intercalated counter-anions,and incorporating dopants,cavi-ties,and single atoms.In particular,hybridizing LDHs with conductive components or in situ growing them on conductive substrates to produce freestanding electrodes can further enhance their intrinsic catalytic activity.A brief discussion on future research directions and prospects is also summarized.展开更多
Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel ce...Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.展开更多
基金supported in part by the WPIMANA,Ministry of Education,Culture,Sports,Science and TechnologyCREST of the Japan Science and Technology Agency(JST)(Grant No.JPMJCR17N1)the support from JSPS KAKENNHI grant 15H02004 and 18H03869.
文摘Layered double hydroxides(LDHs)have attracted tremendous research interest in widely spreading applications.Most notably,transition-metal-bearing LDHs are expected to serve as highly active electrocatalysts for oxygen evolution reaction(OER)due to their layered structure combined with versatile com-positions.Furthermore,reducing the thickness of platelet LDH crystals to nanometer or even molecular scale via cleavage or delamination provides an important clue to enhance the activity.In this review,recent progresses on rational design of LDH nanosheets are reviewed,including direct synthesis via traditional coprecipitation,homogeneous precipitation,and newly developed topochemical oxidation as well as chemical exfoliation of parent LDH crystals.In addition,diverse strategies are introduced to modulate their electrochemical activity by tuning the composition of host metal cations and intercalated counter-anions,and incorporating dopants,cavi-ties,and single atoms.In particular,hybridizing LDHs with conductive components or in situ growing them on conductive substrates to produce freestanding electrodes can further enhance their intrinsic catalytic activity.A brief discussion on future research directions and prospects is also summarized.
基金supported by the National Key Research and Development Program of China(2017YFB0102900 and 2016YFB0101201)the National Natural Science Foundation of China(51971094,21476088 and 21776104)the Guangdong Provincial Department of Science and Technology(2015A030312007)。
文摘Highly active and robust electrocatalysts are desired for proton exchange membrane fuel cells.Pt-based intermetallic compounds(IMCs) have been recognized as one of the most promising low-platinum catalysts for fuel cells(FCs).Herein,we report a high-performance IMCs by anchoring ordered PtCoNi ternary nanoparticles on the N,Co and Ni co-doped dodecahedral mesoporous carbon(DMC).While the introduced Co and Ni participate in the formation of PtCoNi IMCs,some of them are doped in the mesoporous carbon and coordinated by N to form Co-N_(y)/Ni-N_(z)dual active centers,which further enhances the electrocatalytic activity towards oxygen reduction reaction.Moreover,the addition of Ni results in a negative shift of the d-band center of Pt as compared to the Pt/DMC and Pt_(3)Co/DMC,making it easier to adsorb oxygen on the surface.As expected,our optimal sample Pt_(3)Co_(0.7)Ni_(0.3)/DMC exhibits excellent performance with mass activity and specific activity of 1.32 A mgPt-1and 1.98 mA cm^(-2)at 0.9 V,which are 7.33and 6.19 times that of commercial Pt/C,respectively.The Pt_(3)Co_(0.7)Ni_(0.3)/DMC also reveals much better cathodic performance in an H2-air single fuel cell than commercial Pt/C catalyst with a power density of0.802 W cm^(-2).This work provides critical sights into constructing efficient catalysts by ternary intermetallic strategy and synergetic effect between active components and support.
