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Effect of Carbon Support Capping Agent Amount and Pd NPs Size for Bio-Adipic Acid Production from Muconic Acid and Sodium Muconate

机译:碳载体封端剂用量和Pd NPs尺寸对粘康酸和粘康酸钠生产生物己二酸的影响

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摘要

The effect of support, stabilizing agent, and Pd nanoparticles (NPs) size was studied for sodium muconate and t,t-muconic acid hydrogenation to bio-adipic acid. Three different activated carbons (AC) were used (Norit, KB, and G60) and carbon morphology did not affect the substrate conversion, but it greatly influenced the adipic acid yield. 1% Pd/KB Darco catalyst, which has the highest surface area and Pd surface exposure, and the smallest NPs size displayed the highest activity. Furthermore, the effect of the amount of the protective agent was studied varying metal/protective agent weight ratios in the range of 1/0.00–1/1.20, using KB as the chosen support. For sodium muconate reduction 1% Pd/KB_1.2 catalyst gave the best results in terms of activity (0.73 s ), conversion, and adipic acid yield (94.8%), while for t,t-muconic acid hydrogenation the best activity result (0.85 s ) was obtained with 1% Pd/KB_0.0 catalyst. Correlating the results obtained from XPS and TEM analyses with catalytic results, we found that the amount of PVA (polyvinyl alcohol) influences mean Pd NPs size, Pd(0)/Pd(II) ratio, and Pd surface exposure. Pd(0)/Pd(II) ratio and Pd NPs size affected adipic acid yield and activity during sodium muconate hydrogenation, respectively, while adipic acid yield was related by exposed Pd amount during t,t-muconic acid hydrogenation. The synthesized catalysts showed higher activity than commercial 5% Pd/AC.
机译:研究了载体,稳定剂和钯纳米颗粒(NPs)大小对粘液酸钠和叔丁基粘康酸加氢生成己二酸的影响。使用了三种不同的活性炭(AC)(Norit,KB和G60),碳形态并不影响底物转化率,但它极大地影响了己二酸的收率。 1%Pd / KB Darco催化剂具有最高的表面积和Pd表面暴露,最小的NPs活性最高。此外,使用KB作为选择的载体,研究了在金属保护剂重量比在1 / 0.00-1 / 1.20范围内变化时保护剂用量的影响。就粘胶酸钠的还原而言,在活性(0.73 s),转化率和己二酸产率(94.8%)方面,1%Pd / KB_1.2催化剂给出了最佳结果,而对于t,t-粘康酸加氢而言,其活性最好(用1%Pd / KB_0.0催化剂获得0.85 s)。将XPS和TEM分析获得的结果与催化结果进行关联,我们发现PVA(聚乙烯醇)的量会影响平均Pd NPs大小,Pd(0)/ Pd(II)比率和Pd表面暴露。 Pd(0)/ Pd(II)的比值和Pd NPs的大小分别影响粘液酸钠氢化过程中己二酸的产率和活性,而己二酸产率与t,t-粘康酸氢化过程中暴露的Pd量有关。合成的催化剂显示出比市售的5%Pd / AC高的活性。

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