{"title":"竹浆衍生的掺杂 N、P 的分层多孔碳纤维作为还原 4-硝基苯酚的高效碳催化剂","authors":"Liyun Zhang, Weihai Zhou, Yongle Cao, Heng Zhang, Wancheng Zhu","doi":"10.1007/s42823-024-00758-6","DOIUrl":null,"url":null,"abstract":"<div><p>For metal-free carbocatalysts, heteroatom doping and hierarchically porous structure are the significant factors to improve their catalytic performances. Herein, N-, P-co-doped hierarchically porous carbon fiber (NPC–2–800) was prepared by pyrolyzing bamboo pulp in combination with (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> and activator K<sub>2</sub>CO<sub>3</sub>. It was found that (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> not only provides N and P atoms, but also significantly affect the morphology and pore structure of the porous carbon. An appropriate dosage of (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> facilitates the formation of hierarchically porous carbon fiber in NPC-2–800. Whereas, the carbon fragments with only micropores were obtained in absence of (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub>. The hierarchical porosity and the co-doping of N and P atoms in the NPC-2–800 contribute to its outstanding catalytic performances in the 4-Nitrophenol (4-NP) reduction assisted by NaBH<sub>4</sub>. The NPC-2–800 exhibits an attractive turnover frequency (TOF) value of 4.29 × 10<sup>–4</sup> mmol mg<sup>−1</sup> min<sup>−1</sup>, a low activation energy (<i>E</i><sub>a</sub>) of 24.76 kJ/mol, and an acceptable recyclability for 7 cycles without obvious decrease in activity. Kinetics analyses suggest that the 4-NP reduction proceeds through the Langmuir–Hinshelwood model. In addition, the NPC-2–800 can also efficiently catalyze the 2-NP and 3-NP reduction. Moreover, in the real water body, the NPC-2–800 also showed superior catalytic activity to catalyze 4-NP reduction. This study provides an efficient catalyst for pollutant conversion and elimination as well as guidelines for designing versatile carbon-based catalysts.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":506,"journal":{"name":"Carbon Letters","volume":"34 8","pages":"2137 - 2148"},"PeriodicalIF":5.5000,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"N-, P-co-doped hierarchically porous carbon fiber derived from bamboo pulp as efficient carbocatalyst for reduction of 4-nitrophenol\",\"authors\":\"Liyun Zhang, Weihai Zhou, Yongle Cao, Heng Zhang, Wancheng Zhu\",\"doi\":\"10.1007/s42823-024-00758-6\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>For metal-free carbocatalysts, heteroatom doping and hierarchically porous structure are the significant factors to improve their catalytic performances. Herein, N-, P-co-doped hierarchically porous carbon fiber (NPC–2–800) was prepared by pyrolyzing bamboo pulp in combination with (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> and activator K<sub>2</sub>CO<sub>3</sub>. It was found that (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> not only provides N and P atoms, but also significantly affect the morphology and pore structure of the porous carbon. An appropriate dosage of (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub> facilitates the formation of hierarchically porous carbon fiber in NPC-2–800. Whereas, the carbon fragments with only micropores were obtained in absence of (NH<sub>4</sub>)<sub>2</sub>HPO<sub>4</sub>. The hierarchical porosity and the co-doping of N and P atoms in the NPC-2–800 contribute to its outstanding catalytic performances in the 4-Nitrophenol (4-NP) reduction assisted by NaBH<sub>4</sub>. The NPC-2–800 exhibits an attractive turnover frequency (TOF) value of 4.29 × 10<sup>–4</sup> mmol mg<sup>−1</sup> min<sup>−1</sup>, a low activation energy (<i>E</i><sub>a</sub>) of 24.76 kJ/mol, and an acceptable recyclability for 7 cycles without obvious decrease in activity. Kinetics analyses suggest that the 4-NP reduction proceeds through the Langmuir–Hinshelwood model. In addition, the NPC-2–800 can also efficiently catalyze the 2-NP and 3-NP reduction. Moreover, in the real water body, the NPC-2–800 also showed superior catalytic activity to catalyze 4-NP reduction. This study provides an efficient catalyst for pollutant conversion and elimination as well as guidelines for designing versatile carbon-based catalysts.</p><h3>Graphical abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":506,\"journal\":{\"name\":\"Carbon Letters\",\"volume\":\"34 8\",\"pages\":\"2137 - 2148\"},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2024-06-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s42823-024-00758-6\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Letters","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s42823-024-00758-6","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
N-, P-co-doped hierarchically porous carbon fiber derived from bamboo pulp as efficient carbocatalyst for reduction of 4-nitrophenol
For metal-free carbocatalysts, heteroatom doping and hierarchically porous structure are the significant factors to improve their catalytic performances. Herein, N-, P-co-doped hierarchically porous carbon fiber (NPC–2–800) was prepared by pyrolyzing bamboo pulp in combination with (NH4)2HPO4 and activator K2CO3. It was found that (NH4)2HPO4 not only provides N and P atoms, but also significantly affect the morphology and pore structure of the porous carbon. An appropriate dosage of (NH4)2HPO4 facilitates the formation of hierarchically porous carbon fiber in NPC-2–800. Whereas, the carbon fragments with only micropores were obtained in absence of (NH4)2HPO4. The hierarchical porosity and the co-doping of N and P atoms in the NPC-2–800 contribute to its outstanding catalytic performances in the 4-Nitrophenol (4-NP) reduction assisted by NaBH4. The NPC-2–800 exhibits an attractive turnover frequency (TOF) value of 4.29 × 10–4 mmol mg−1 min−1, a low activation energy (Ea) of 24.76 kJ/mol, and an acceptable recyclability for 7 cycles without obvious decrease in activity. Kinetics analyses suggest that the 4-NP reduction proceeds through the Langmuir–Hinshelwood model. In addition, the NPC-2–800 can also efficiently catalyze the 2-NP and 3-NP reduction. Moreover, in the real water body, the NPC-2–800 also showed superior catalytic activity to catalyze 4-NP reduction. This study provides an efficient catalyst for pollutant conversion and elimination as well as guidelines for designing versatile carbon-based catalysts.
期刊介绍:
Carbon Letters aims to be a comprehensive journal with complete coverage of carbon materials and carbon-rich molecules. These materials range from, but are not limited to, diamond and graphite through chars, semicokes, mesophase substances, carbon fibers, carbon nanotubes, graphenes, carbon blacks, activated carbons, pyrolytic carbons, glass-like carbons, etc. Papers on the secondary production of new carbon and composite materials from the above mentioned various carbons are within the scope of the journal. Papers on organic substances, including coals, will be considered only if the research has close relation to the resulting carbon materials. Carbon Letters also seeks to keep abreast of new developments in their specialist fields and to unite in finding alternative energy solutions to current issues such as the greenhouse effect and the depletion of the ozone layer. The renewable energy basics, energy storage and conversion, solar energy, wind energy, water energy, nuclear energy, biomass energy, hydrogen production technology, and other clean energy technologies are also within the scope of the journal. Carbon Letters invites original reports of fundamental research in all branches of the theory and practice of carbon science and technology.