Advancing clean energy technologies demands efficient and durable electrode catalysts for solid oxide cells(SOCs).Despite their exceptional catalytic properties,Pt-based materials face critical challenges in high-temp...Advancing clean energy technologies demands efficient and durable electrode catalysts for solid oxide cells(SOCs).Despite their exceptional catalytic properties,Pt-based materials face critical challenges in high-temperature applications owing to particle agglomeration and cost constraints.Here,we demonstrate a rational design strategy utilizing controlled in situ exsolution to create strongly anchored PtSn nanoalloys on oxygen-deficient PrBaMn_(1.8)Pt_(0.1)Sn_(0.1)O_(5+δ)(L-PBMPtSn)perovskite oxide.Through precise compositional engineering and structural control,we achieved a uniform dispersion of PtSn nanoparticles with unique socket-like interfaces that prevent agglomeration while maintaining high catalytic accessibility.The optimized electrode demonstrates remarkable bifunctional performance,achieving a current density of 1.6 A cm^(-2)at 1.8 V for CO_(2)electrolysis and a maximum power density of 316 mW cm^(-2)for fuel cell operation at 800℃.More significantly,the electrode exhibits exceptional stability with only 9.6%performance degradation over 100 h of operation,which is a substantial improvement over conventional electrodes.Our findings establish a new paradigm for designing high-performance SOC electrodes through the controlled exsolution of precious metal alloys,offering broader implications for catalyst design in high-temperature electrochemical systems.展开更多
用微型催化反应装置结合X射线衍射(XRD)、H2化学吸附、NH3吸附-程序升温脱附(NH3-TPD)和H2-程序升温还原等多种物理化学手段研究了丙烷脱氢负载型Pt Sn Na/SUZ-4催化剂中Na+助剂组分的作用。结果表明,Na+组分可中和SUZ-4载体表面的强酸...用微型催化反应装置结合X射线衍射(XRD)、H2化学吸附、NH3吸附-程序升温脱附(NH3-TPD)和H2-程序升温还原等多种物理化学手段研究了丙烷脱氢负载型Pt Sn Na/SUZ-4催化剂中Na+助剂组分的作用。结果表明,Na+组分可中和SUZ-4载体表面的强酸中心、提高催化剂的Pt金属分散度、抑制脱氢产物的裂解和积炭的生成,从而提高催化剂的丙烷脱氢选择性和反应稳定性。但是过量Na+组分的存在会削弱Sn物种与载体之间的相互作用,使其易被还原,导致催化剂丙烷脱氢活性显著下降。展开更多
A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarc...A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarchical ZSM-5 catalysts was achieved via the loading of Pt and Sn species onto the hierarchical ZSM-5 catalysts that are obtained through a desilication of conventional ZSM-5.The PtSn/hierarchical ZSM-5 catalysts were fully characterized by XRD,N_(2) adsorption,STEM,XPS,and CO-IR techniques,which reveals that highly dispersed PtSn bimetallic nanoparticles are enclosed into mesopores of hierarchical ZSM-5.The catalytic performance of PtSn/hierarchical ZSM-5 is greatly affected by the concentrations of alkali solution in the desilication process and Sn/Pt ratios in PtSn bimetallic particles.The PtSn1.00/ZSM-5(0.8)catalyst shows the highest efficiency in propane dehydrogenation,which gives an initial conversion of 46%and selectivity of 98%at 570℃.The high efficiency in these PtSn/hierarchical ZSM-5 catalysts for propane dehydrogenation is mainly ascribed to the confinement of PtSn particles in the mesopores of hierarchical ZSM-5 zeolite.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22272081 and 52473235)Postgraduate Research and Practice Innovation Program of Jiangsu Province(No.KYCX24_1527)National Research Foundation of Korea(NRF)grant funded by the Korea governement(MSIT)(No.RS-2024-00347253)
文摘Advancing clean energy technologies demands efficient and durable electrode catalysts for solid oxide cells(SOCs).Despite their exceptional catalytic properties,Pt-based materials face critical challenges in high-temperature applications owing to particle agglomeration and cost constraints.Here,we demonstrate a rational design strategy utilizing controlled in situ exsolution to create strongly anchored PtSn nanoalloys on oxygen-deficient PrBaMn_(1.8)Pt_(0.1)Sn_(0.1)O_(5+δ)(L-PBMPtSn)perovskite oxide.Through precise compositional engineering and structural control,we achieved a uniform dispersion of PtSn nanoparticles with unique socket-like interfaces that prevent agglomeration while maintaining high catalytic accessibility.The optimized electrode demonstrates remarkable bifunctional performance,achieving a current density of 1.6 A cm^(-2)at 1.8 V for CO_(2)electrolysis and a maximum power density of 316 mW cm^(-2)for fuel cell operation at 800℃.More significantly,the electrode exhibits exceptional stability with only 9.6%performance degradation over 100 h of operation,which is a substantial improvement over conventional electrodes.Our findings establish a new paradigm for designing high-performance SOC electrodes through the controlled exsolution of precious metal alloys,offering broader implications for catalyst design in high-temperature electrochemical systems.
文摘用微型催化反应装置结合X射线衍射(XRD)、H2化学吸附、NH3吸附-程序升温脱附(NH3-TPD)和H2-程序升温还原等多种物理化学手段研究了丙烷脱氢负载型Pt Sn Na/SUZ-4催化剂中Na+助剂组分的作用。结果表明,Na+组分可中和SUZ-4载体表面的强酸中心、提高催化剂的Pt金属分散度、抑制脱氢产物的裂解和积炭的生成,从而提高催化剂的丙烷脱氢选择性和反应稳定性。但是过量Na+组分的存在会削弱Sn物种与载体之间的相互作用,使其易被还原,导致催化剂丙烷脱氢活性显著下降。
基金supports of the National Natural Science Foundation of China(21878050,22178062)Foundation of State Key Labora-tory of Coal Conversion(J21-22-620)Green Petrochemical Engineering Base of Intelligence Introduction for Innovation(111 Project D17005)are gratefully acknowledged.
文摘A series of PtSn/hierarchical ZSM-5 catalysts were developed for propane dehydrogenation,in which the PtSn bimetallic particles are confined in the mesopores of hierarchical ZSM-5 zeolite.The synthesis of PtSn/hierarchical ZSM-5 catalysts was achieved via the loading of Pt and Sn species onto the hierarchical ZSM-5 catalysts that are obtained through a desilication of conventional ZSM-5.The PtSn/hierarchical ZSM-5 catalysts were fully characterized by XRD,N_(2) adsorption,STEM,XPS,and CO-IR techniques,which reveals that highly dispersed PtSn bimetallic nanoparticles are enclosed into mesopores of hierarchical ZSM-5.The catalytic performance of PtSn/hierarchical ZSM-5 is greatly affected by the concentrations of alkali solution in the desilication process and Sn/Pt ratios in PtSn bimetallic particles.The PtSn1.00/ZSM-5(0.8)catalyst shows the highest efficiency in propane dehydrogenation,which gives an initial conversion of 46%and selectivity of 98%at 570℃.The high efficiency in these PtSn/hierarchical ZSM-5 catalysts for propane dehydrogenation is mainly ascribed to the confinement of PtSn particles in the mesopores of hierarchical ZSM-5 zeolite.
