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A Carbon Catalyst Co-Doped with P and N for Efficient and Selective Oxidation of 5-Hydroxymethylfurfural into 2,5-Diformylfuran.
ChemSusChem ( IF 7.5 ) Pub Date : 2020-08-17 , DOI: 10.1002/cssc.202001525 Huifa Zhang 1 , James H Clark 2 , Tong Geng 1 , Huixian Zhang 3 , Fahai Cao 1
ChemSusChem ( IF 7.5 ) Pub Date : 2020-08-17 , DOI: 10.1002/cssc.202001525 Huifa Zhang 1 , James H Clark 2 , Tong Geng 1 , Huixian Zhang 3 , Fahai Cao 1
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A newly designed N and P co‐doped carbon material has been developed to catalyze the conversion of 5‐hydroxymethylfurfural (HMF) to 2,5‐furandialdehyde (DFF) with unprecedented yield and selectivity and demonstrating a synergistic effect between the heteroatoms. The desired catalyst was first synthesized via a pyrolysis method using urea as the nitrogen and carbon source followed by calcination with phytic acid solution as the phosphorus source. The mass ratio of phytic acid to C3N4 and calcination temperature were varied to investigate their effects on catalyst synthesis and microstructure as well as subsequent catalytic activity in simple reaction systems under oxygen. The effect of reaction conditions on the final HMF conversion and DFF selectivity were also investigated systematically. The P−C−N‐5‐800 catalyst obtained with the optimized annealing temperature of 800 °C and mass ratio of phytic acid/C3N4 of 5 enabled a 99.5 % DFF yield at 120 °C for 9 h under 10 bar oxygen pressure, being the highest among any reported metal‐free heterogeneous catalyst to date. The excellent performance of P−C−N‐5‐800 could be ascribed to the synergy between N and P heteroatoms as well as the high content of graphitic‐N and the P−C species within the carbon structure. Reusability studies show that the P−C−N‐5‐800 catalyst was stable and reusable without deactivation. These results strongly suggest that P−C−N‐5‐800 is a promising catalyst for large‐scale production of DFF in a green manner.
中文翻译：
共掺杂P和N的碳催化剂，用于将5-羟基甲基糠醛有效和选择性地氧化为2,5-二甲酰呋喃。
已开发出一种新设计的氮和磷共掺杂碳材料，以前所未有的收率和选择性催化5-羟甲基糠醛（HMF）转化为2,5-呋喃二醛（DFF），并证明了杂原子之间的协同作用。首先通过热解法使用尿素作为氮和碳源来合成所需的催化剂，然后以植酸溶液作为磷源进行煅烧。植酸与C 3 N 4的质量比改变煅烧温度和煅烧温度以研究它们对催化剂合成和微观结构以及随后在氧气中的简单反应体系中的催化活性的影响。还系统地研究了反应条件对最终HMF转化率和DFF选择性的影响。以最佳退火温度800°C和植酸/ C 3 N 4的质量比获得的P-C-N-5-800催化剂仅有5个样品能在10 bar氧气压力下于120°C加热9 h达到99.5％的DFF产率，是迄今为止报道的无金属多相催化剂中最高的。P-C-N-5-800的优异性能可归因于N和P杂原子之间的协同作用，以及石墨碳和碳结构中P-C物种的高含量。可重用性研究表明，PCN-5-800催化剂稳定且可重用而不会失活。这些结果强烈表明，PC-N-5-800是一种以绿色方式大规模生产DFF的有希望的催化剂。
更新日期：2020-08-17
中文翻译：
共掺杂P和N的碳催化剂，用于将5-羟基甲基糠醛有效和选择性地氧化为2,5-二甲酰呋喃。
已开发出一种新设计的氮和磷共掺杂碳材料，以前所未有的收率和选择性催化5-羟甲基糠醛（HMF）转化为2,5-呋喃二醛（DFF），并证明了杂原子之间的协同作用。首先通过热解法使用尿素作为氮和碳源来合成所需的催化剂，然后以植酸溶液作为磷源进行煅烧。植酸与C 3 N 4的质量比改变煅烧温度和煅烧温度以研究它们对催化剂合成和微观结构以及随后在氧气中的简单反应体系中的催化活性的影响。还系统地研究了反应条件对最终HMF转化率和DFF选择性的影响。以最佳退火温度800°C和植酸/ C 3 N 4的质量比获得的P-C-N-5-800催化剂仅有5个样品能在10 bar氧气压力下于120°C加热9 h达到99.5％的DFF产率，是迄今为止报道的无金属多相催化剂中最高的。P-C-N-5-800的优异性能可归因于N和P杂原子之间的协同作用，以及石墨碳和碳结构中P-C物种的高含量。可重用性研究表明，PCN-5-800催化剂稳定且可重用而不会失活。这些结果强烈表明，PC-N-5-800是一种以绿色方式大规模生产DFF的有希望的催化剂。
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