Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacit...Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacities,perovskite‐type redox catalysts have attracted significant attention in this regard.In the present study,the perovskite series La1‐xCaxMn1‐yAlyO3(x,y=0.2,0.4,0.6,or0.8)was fabricated using a modified Pechini method and comprehensively investigated to determine the applicability of these materials to solar H2production via two‐step thermochemical water splitting.The thermochemical redox behaviors of these perovskites were optimized by doping at either the A(Ca)or B(Al)sites over a broad range of substitution values,from0.2to0.8.Through this doping,a highly efficient perovskite(La0.6Ca0.4Mn0.6Al0.4O3)was developed,which yielded a remarkable H2production rate of429μmol/g during two‐step thermochemical H2O splitting,going between1400and1000°C.Moreover,the performance of the optimized perovskite was found to be eight times higher than that of the benchmark catalyst CeO2under the same experimental conditions.Furthermore,these perovskites also showed impressive catalytic stability during two‐step thermochemical cycling tests.These newly developed La1‐xCaxMn1‐yAlyO3redox catalysts appear to have great potential for future practical applications in thermochemical solar fuel production.展开更多
基金supported by the Australian Research Council(FT120100913)the National Natural Science Foundation of China(51372248,51432009)~~
文摘Solar‐driven thermochemical water splitting represents one efficient route to the generation of H2as a clean and renewable fuel.Due to their outstanding catalytic abilities and promising solar fuel production capacities,perovskite‐type redox catalysts have attracted significant attention in this regard.In the present study,the perovskite series La1‐xCaxMn1‐yAlyO3(x,y=0.2,0.4,0.6,or0.8)was fabricated using a modified Pechini method and comprehensively investigated to determine the applicability of these materials to solar H2production via two‐step thermochemical water splitting.The thermochemical redox behaviors of these perovskites were optimized by doping at either the A(Ca)or B(Al)sites over a broad range of substitution values,from0.2to0.8.Through this doping,a highly efficient perovskite(La0.6Ca0.4Mn0.6Al0.4O3)was developed,which yielded a remarkable H2production rate of429μmol/g during two‐step thermochemical H2O splitting,going between1400and1000°C.Moreover,the performance of the optimized perovskite was found to be eight times higher than that of the benchmark catalyst CeO2under the same experimental conditions.Furthermore,these perovskites also showed impressive catalytic stability during two‐step thermochemical cycling tests.These newly developed La1‐xCaxMn1‐yAlyO3redox catalysts appear to have great potential for future practical applications in thermochemical solar fuel production.
