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Late-Transition-Metal-Modified β-Mo2C Catalysts for Enhanced Hydrogenation during Guaiacol Deoxygenation
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2017-11-08 00:00:00 , DOI: 10.1021/acssuschemeng.7b02544
Frederick G. Baddour 1 , Vanessa A. Witte 1 , Connor P. Nash 1 , Michael B. Griffin 1 , Daniel A. Ruddy 1 , Joshua A. Schaidle 1
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2017-11-08 00:00:00 , DOI: 10.1021/acssuschemeng.7b02544
Frederick G. Baddour 1 , Vanessa A. Witte 1 , Connor P. Nash 1 , Michael B. Griffin 1 , Daniel A. Ruddy 1 , Joshua A. Schaidle 1
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Molybdenum carbide has been identified as a promising bifunctional catalyst in the deoxygenation of a variety of pyrolysis vapor model compounds. Although high deoxygenation activity has been demonstrated, complementary hydrogenation activity has been limited, especially for lignin-derived, aromatic model compounds. The ability to control the relative site densities of acidic and hydrogenation functionalities represents a catalyst design challenge for these materials with the goal to improve hydrogenation activity under ex situ catalytic fast pyrolysis (CFP) conditions. Here we demonstrate that the addition of Pt and Ni to β-Mo2C resulted in an increase in the H*-site density with only a minor decrease in the acid-site density. In contrast, the addition of Pd did not significantly alter the H*- or acid-site densities. High conversions (>94%) and high selectivities to 0-oxygen products (>80%) were observed in guaiacol deoxygenation under ex situ CFP conditions (350 °C and 0.44 MPa H2) for all catalysts. Pt addition resulted in the greatest deoxygenation, and site-time yields to hydrogenated products over the Pt/Mo2C catalyst were increased to 0.048 s–1 compared to 0.015–0.019 s–1 for all other catalysts. The Pt/Mo2C catalyst demonstrated the highest hydrogenation performance, but modification with Ni also significantly enhanced hydrogenation performance, representing a promising lower-cost alternative.
中文翻译：
迟-过渡金属改性的β-沫2 C催化剂用于氢化增强愈创木酚脱氧期间
碳化钼在各种热解蒸气模型化合物的脱氧反应中被认为是一种有前途的双功能催化剂。尽管已证明了高脱氧活性，但互补的氢化活性却受到限制，尤其是对于木质素衍生的芳族模型化合物而言。控制酸性和氢化功能的相对位点密度的能力代表了这些材料的催化剂设计挑战，目的是提高在异位催化快速热解（CFP）条件下的氢化活性。在这里，我们表明，加入Pt和Ni成β钼2C导致H *位密度增加，而酸位密度仅轻微降低。相反，Pd的添加不会显着改变H *-或酸性位点的密度。高的转化率（> 94％）和高选择性为0-氧产物（> 80％）在愈创木酚脱氧观察下易地CFP条件（350℃，0.44兆帕ħ 2）对于所有的催化剂。Pt的添加导致最大的脱氧作用，Pt / Mo 2 C催化剂上氢化产物的现场时间收率提高至0.048 s –1，而所有其他催化剂为0.015–0.019 s –1。铂/钼2C催化剂显示出最高的氢化性能，但用Ni改性也显着增强了氢化性能，代表了一种有前途的低成本替代品。
更新日期：2017-11-08
中文翻译：
迟-过渡金属改性的β-沫2 C催化剂用于氢化增强愈创木酚脱氧期间
碳化钼在各种热解蒸气模型化合物的脱氧反应中被认为是一种有前途的双功能催化剂。尽管已证明了高脱氧活性，但互补的氢化活性却受到限制，尤其是对于木质素衍生的芳族模型化合物而言。控制酸性和氢化功能的相对位点密度的能力代表了这些材料的催化剂设计挑战，目的是提高在异位催化快速热解（CFP）条件下的氢化活性。在这里，我们表明，加入Pt和Ni成β钼2C导致H *位密度增加，而酸位密度仅轻微降低。相反，Pd的添加不会显着改变H *-或酸性位点的密度。高的转化率（> 94％）和高选择性为0-氧产物（> 80％）在愈创木酚脱氧观察下易地CFP条件（350℃，0.44兆帕ħ 2）对于所有的催化剂。Pt的添加导致最大的脱氧作用，Pt / Mo 2 C催化剂上氢化产物的现场时间收率提高至0.048 s –1，而所有其他催化剂为0.015–0.019 s –1。铂/钼2C催化剂显示出最高的氢化性能，但用Ni改性也显着增强了氢化性能，代表了一种有前途的低成本替代品。
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