太阳能热化学分解水是一种高效生产清洁和可再生氢能源的方法.由于出色的催化活性和太阳能燃料生产能力,钙钛矿型的催化剂在热化学领域引起了强烈关注.我们采用改良的Pechini法合成了一系列钙铝掺杂的镧锰钙钛矿并系统考察了其在两步法热化学分解水中的产氢表现.为了优化热化学催化性能,我们进行了镧锰钙钛矿A,B位上钙和铝的掺杂量(从0.2到0.8)的详细考察.通过调整掺杂比例,得到了一种极其高效的钙钛矿催化剂La0.6Ca0.4Mn0.6Al0.4O3.当两步法热化学分解水在1400和1000℃之间,La0.6Ca0.4Mn0.6Al0.4O3取得了429μmol/g的出色产氢表现,比同等条件下基准催化剂氧化铈产氢结果高出8倍.与此同时,钙铝掺杂镧锰钙钛矿在两步法热化学循环测试中展现出极其稳定的催化活性.因此,这种新颖的钙铝掺杂镧锰钙钛矿具备巨大的潜质用于未来热化学太阳能燃料的实际生产.%Solar-driven thermochemical water splitting represents one efficient route to the generation of H2 as 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, or 0.8) was fabricated using a modified Pechini method and comprehensively investigated to determine the applicability of these materials to solar H2 productionvia 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, from 0.2 to 0.8. Through this doping, a highly efficient perovskite (La0.6Ca0.4Mn0.6Al0.4O3) was developed, which yielded a remarkable H2 production rate of 429 μmol/g during two-step thermochemical H2O splitting, going between 1400 and 1000 ℃. Moreover, the performance of the optimized perovskite was found to be eight times higher than that of the benchmark catalyst CeO2 under the same experimental conditions. Further-more, these perovskites also showed impressive catalytic stability during two-step thermochemical cycling tests. These newly developed La1-xCaxMn1-yAlyO3 redox catalysts appear to have great poten-tial for future practical applications in thermochemical solar fuel production.
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