Synthesis of lignin-derived nitrogen-doped carbon as a novel catalyst for 4-NP reduction evaluation.
Synthesis of lignin-derived nitrogen-doped carbon as a novel catalyst for 4-NP reduction evaluation.
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木质素衍生的氮掺杂碳的合成作为4-NP还原评价的新型催化剂
DOI：
10.1038/s41598-020-76039-9
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发表时间：
2020-11-18
影响因子：
4.6
通讯作者：
Chen T
中科院分区：
文献类型：
--
作者：
Liu Y;Xu H;Yu H;Yang H;Chen T
本研究以木质素为碳源，g-C3 N4为牺牲模板和氮源，制备了氮掺杂碳材料。采用TEM、XRD、FT-IR、拉曼、XPS和BET等测试技术对所制备的NC的结构进行了表征。有吸引力的是，NC已被证明可有效地使用NaBH 4作为氢供体将4-硝基苯酚（4-NP）还原为4-氨基苯酚（4-AP），具有高表观速率常数（kapp = 4.77 min−1）和比质量活性（s = 361 mol kgcat−1 h−1），这些值上级于文献中先前报道的催化剂。密度泛函理论（DFT）计算结果表明，四种氮掺杂剂均能改变相邻碳原子的电子结构，并对催化性能产生影响，但石墨态氮物种对4-NP吸附和催化还原的贡献更大.此外，根据XPS和DFT数据，提出了该转移加氢反应的初步机理。令人惊讶的是，NC具有优异的稳定性和连续六次运行的可重复使用性，而不会损失催化活性。这些发现开辟了一个前景，工程木质素衍生的NC作为加氢反应的无金属催化剂。
In this study, nitrogen-doped carbon (NC) was fabricated using lignin as carbon source and g-C3N4 as sacrificial template and nitrogen source. The structural properties of as-prepared NC were characterized by TEM, XRD, FT-IR, Raman, XPS and BET techniques. Attractively, NC has proved efficient for reducing 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) using NaBH4 as hydrogen donor with high apparent rate constant (kapp = 4.77 min−1) and specific mass activity (s = 361 mol kgcat−1 h−1), which values are superior to the previously reported catalysts in the literature. Density functional theory (DFT) calculations demonstrate that four kinds of N dopants can change the electronic structure of the adjacent carbon atoms and contribute to their catalytic properties dependant on N species, however, graphitic N species has much greater contribution to 4-NP adsorption and catalytic reduction. Furthermore, The preliminary mechanism of this transfer hydrogenation reaction over as-prepared NC is proposed on the basis of XPS and DFT data. Astoundingly, NC has excellent stability and reusability of six consecutive runs without loss of catalytic activity. These findings open up a vista to engineer lignin-derived NC as metal-free catalyst for hydrogenation reaction.
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影响因子：
15
作者：
Błoński P;Tuček J;Sofer Z;Mazánek V;Petr M;Pumera M;Otyepka M;Zbořil R
通讯作者：
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影响因子：
17.1
作者：
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通讯作者：
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影响因子：
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作者：
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影响因子：
15
作者：
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通讯作者：
Qiao, Shi Zhang
影响因子：
4.9
作者：
Ciganda, Roberto;Li, Na;Astruc, Didier
通讯作者：
Astruc, Didier