开发用于木质素增值的高效无金属催化剂是必不可少的,但具有挑战性。在这项研究中,采用具有成本效益的策略来合成P,通过水热和碳化过程的N共掺杂碳催化剂。该催化剂有效地裂解了α-O-4,β-O-4和4-O-5木质素键,正如模型化合物所证明的那样。在不同的碳化温度下制备了各种催化剂,并使用XRD,拉曼,FTIR,XPS,NH3-TPD,和HRTEM。归因于较高的酸度,P5NC-500催化剂表现出最好的催化活性,在水中使用H2O2作为氧化剂。此外,这种无金属技术有效地转化了模拟木质素生物油,包含所有三个链接,变成有价值的单体。密度泛函理论计算提供了对反应机理的见解,表明P5NC-500中的P-O-H位点和CN催化剂中的N-C-O-H对底物和氧化剂的活化。此外,催化剂的可回收性和水利用率增强了其环境相容性,提供了一个高度可持续的方法木质素的价值与潜在的应用在各种行业。
Developing efficient metal-free catalysts for
lignin valorization is essential but challenging. In this study, a cost-effective strategy is employed to synthesize a P, N co-doped carbon catalyst through hydrothermal and carbonization processes. This catalyst effectively cleaved α-O-4, β-O-4, and 4-O-5
lignin linkages, as demonstrated with model compounds. Various catalysts were prepared at different carbonization temperatures and thoroughly characterized using techniques such as XRD, RAMAN, FTIR, XPS, NH3-TPD, and HRTEM. Attributed to higher acidity, the P5NC-500 catalyst exhibited the best catalytic activity, employing H2O2 as the oxidant in water. Additionally, this metal-free technique efficiently converted simulated
lignin bio-oil, containing all three linkages, into valuable monomers. Density Functional Theory calculations provided insight into the reaction mechanism, suggesting substrate and oxidant activation by P-O-H sites in the P5NC-500, and by N-C-O-H in the CN catalyst. Moreover, the catalyst\'s recyclability and water utilization enhance its environmental compatibility, offering a highly sustainable approach to
lignin valorization with potential applications in various industries.