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Noble-Metal-Free Ni–W–O-Derived Catalysts for High-Capacity Hydrogen Production from Hydrazine Monohydrate
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2020-04-01 , DOI: 10.1021/acssuschemeng.9b07782 Qing Shi 1 , Deng-Xue Zhang 1 , Hui Yin 1 , Yu-Ping Qiu 1 , Liang-Liang Zhou 1 , Chen Chen 1 , Hui Wu 2 , Ping Wang 1
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2020-04-01 , DOI: 10.1021/acssuschemeng.9b07782 Qing Shi 1 , Deng-Xue Zhang 1 , Hui Yin 1 , Yu-Ping Qiu 1 , Liang-Liang Zhou 1 , Chen Chen 1 , Hui Wu 2 , Ping Wang 1
Affiliation
Development of active and earth-abundant catalysts is pivotal to render hydrazine monohydrate (N2H4·H2O) viable as a hydrogen carrier. Herein, we report the synthesis of noble-metal-free Ni–W–O-derived catalysts using a hydrothermal method in combination with reductive annealing treatment. Interestingly, the thus-prepared Ni-based catalysts exhibit remarkably distinct catalytic properties toward N2H4·H2O decomposition depending upon the annealing temperature. From a systematic phase/microstructure/chemical state characterization and the first-principles calculations, we found that the variation of the apparent catalytic properties of these Ni-based catalysts should stem from the formation of different Ni–W alloys with distinct intrinsic activity, selectivity, and distribution state. The thereby chosen Ni–W alloy nanocomposite catalyst prepared under an optimized condition showed high activity, nearly 100% selectivity, and excellent stability toward N2H4·H2O decomposition for hydrogen production. Furthermore, this noble-metal-free catalyst enables rapid hydrogen production from commercially available N2H4·H2O solution with an intriguingly high hydrogen capacity of 6.28 wt % and a satisfactory dynamic response property. These results are inspiring and momentous for promoting the use of the N2H4·H2O-based H2 source systems.
中文翻译:
无贵金属的Ni–W–O衍生的一水合肼高容量制氢催化剂
活性和富含地球的催化剂的开发对于使一水合肼(N 2 H 4 ·H 2 O)能够用作氢载体至关重要。在这里,我们报告了使用水热方法结合还原退火处理合成不含贵金属的Ni–W–O催化剂。有趣的是,如此制备的Ni基催化剂对N 2 H 4 ·H 2表现出明显不同的催化性能。O分解取决于退火温度。通过系统的相/微结构/化学状态表征和第一性原理计算,我们发现这些镍基催化剂的表观催化性能的变化应源自具有不同内在活性,选择性的不同镍-钨合金的形成。 ,以及分配状态。由此选择的在优化条件下制备的Ni-W合金纳米复合催化剂显示出高活性,近100%的选择性以及对制氢过程中N 2 H 4 ·H 2 O分解的优异稳定性。此外,这种不含贵金属的催化剂可从市售的N 2 H 4 ·H快速制氢2 O溶液具有6.28 wt%的极高氢容量和令人满意的动态响应特性。这些结果对于促进使用基于N 2 H 4 ·H 2 O的H 2源系统具有启发性和重大意义。
更新日期:2020-04-01
中文翻译:
无贵金属的Ni–W–O衍生的一水合肼高容量制氢催化剂
活性和富含地球的催化剂的开发对于使一水合肼(N 2 H 4 ·H 2 O)能够用作氢载体至关重要。在这里,我们报告了使用水热方法结合还原退火处理合成不含贵金属的Ni–W–O催化剂。有趣的是,如此制备的Ni基催化剂对N 2 H 4 ·H 2表现出明显不同的催化性能。O分解取决于退火温度。通过系统的相/微结构/化学状态表征和第一性原理计算,我们发现这些镍基催化剂的表观催化性能的变化应源自具有不同内在活性,选择性的不同镍-钨合金的形成。 ,以及分配状态。由此选择的在优化条件下制备的Ni-W合金纳米复合催化剂显示出高活性,近100%的选择性以及对制氢过程中N 2 H 4 ·H 2 O分解的优异稳定性。此外,这种不含贵金属的催化剂可从市售的N 2 H 4 ·H快速制氢2 O溶液具有6.28 wt%的极高氢容量和令人满意的动态响应特性。这些结果对于促进使用基于N 2 H 4 ·H 2 O的H 2源系统具有启发性和重大意义。