{"title":"含氮多壁碳纳米管的简易合成作为氢气进化反应和半咔嗪氧化的无价金属电催化剂","authors":"","doi":"10.1016/j.ijhydene.2024.10.130","DOIUrl":null,"url":null,"abstract":"<div><div>Studies of metal-free carbon nanostructures prove effective in energy and environmental applications due to their molecular tunability and vast chemical space. Herein, we synthesize nitrogen-containing multi-walled carbon nanotubes (N-MWCNTs) via. acid-catalysed incorporation of 3, 4-diaminopyridine into multi-walled carbon nanotubes (MWCNTs), and demonstrating their efficacy in electrocatalytic hydrogen evolution reaction (HER) and semicarbazide (SCB) oxidation for energy and environmental waste management, respectively. Successful synthesis is further confirmed by analysis techniques, i.e. Fourier transform infrared (FTIR) spectral analysis shows the diminishing OH frequency around 3250 cm<sup>−1</sup> in MWCNTs after functionalization and the formation of an O<img>C–NH bond in N-MWCNTs at 1710 cm<sup>−1</sup>. X-ray diffraction (XRD) confirms the incorporation of N-species, while Raman spectroscopic analysis indicates an increase in the I<sub>D</sub>/I<sub>G</sub> ratio MWCNTs (∼1) to N-MWCNTs (∼1.25), suggesting more defective sites in the N-MWCNTs nanocomposite. X-ray photoelectron spectroscopy (XPS) reveals peaks at 399.38, 400.49, and 402.05 eV, attributed to pyridinic-N, aromatic amide-N, and protonated amine groups, respectively. N₂ adsorption-desorption studies shows a high Brunauer-Emmett-Teller (BET) surface area for N-MWCNTs (119.22 m<sup>2</sup>/g) compared to MWCNTs (74.94 m<sup>2</sup>/g). Linear sweep voltammetry (LSV) profiles demonstrate enhanced activity of N-MWCNTs for both HER and SCB oxidation at an ultralow potential of E = −0.55 V vs RHE at 10 mA/cm<sup>2</sup>, with a lower Tafel slope of 108 mV.dec<sup>−1</sup>. Moreover, the electrochemical sensing studies indicates on N-MWCNTs were demonstrating an efficient electron transfer to SCB with the lower detection limit of 0.004 μmol. This work provides carbon-based metal-free electrocatalysts for energy harvesting and environmental management.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Facile synthesis of nitrogen-containing multiwalled carbon nanotubes as a worth metal-free electrocatalyst for hydrogen evolution reaction and semicarbazide oxidation\",\"authors\":\"\",\"doi\":\"10.1016/j.ijhydene.2024.10.130\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Studies of metal-free carbon nanostructures prove effective in energy and environmental applications due to their molecular tunability and vast chemical space. Herein, we synthesize nitrogen-containing multi-walled carbon nanotubes (N-MWCNTs) via. acid-catalysed incorporation of 3, 4-diaminopyridine into multi-walled carbon nanotubes (MWCNTs), and demonstrating their efficacy in electrocatalytic hydrogen evolution reaction (HER) and semicarbazide (SCB) oxidation for energy and environmental waste management, respectively. Successful synthesis is further confirmed by analysis techniques, i.e. Fourier transform infrared (FTIR) spectral analysis shows the diminishing OH frequency around 3250 cm<sup>−1</sup> in MWCNTs after functionalization and the formation of an O<img>C–NH bond in N-MWCNTs at 1710 cm<sup>−1</sup>. X-ray diffraction (XRD) confirms the incorporation of N-species, while Raman spectroscopic analysis indicates an increase in the I<sub>D</sub>/I<sub>G</sub> ratio MWCNTs (∼1) to N-MWCNTs (∼1.25), suggesting more defective sites in the N-MWCNTs nanocomposite. X-ray photoelectron spectroscopy (XPS) reveals peaks at 399.38, 400.49, and 402.05 eV, attributed to pyridinic-N, aromatic amide-N, and protonated amine groups, respectively. N₂ adsorption-desorption studies shows a high Brunauer-Emmett-Teller (BET) surface area for N-MWCNTs (119.22 m<sup>2</sup>/g) compared to MWCNTs (74.94 m<sup>2</sup>/g). Linear sweep voltammetry (LSV) profiles demonstrate enhanced activity of N-MWCNTs for both HER and SCB oxidation at an ultralow potential of E = −0.55 V vs RHE at 10 mA/cm<sup>2</sup>, with a lower Tafel slope of 108 mV.dec<sup>−1</sup>. Moreover, the electrochemical sensing studies indicates on N-MWCNTs were demonstrating an efficient electron transfer to SCB with the lower detection limit of 0.004 μmol. This work provides carbon-based metal-free electrocatalysts for energy harvesting and environmental management.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-10-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Hydrogen Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0360319924043283\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Hydrogen Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0360319924043283","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Facile synthesis of nitrogen-containing multiwalled carbon nanotubes as a worth metal-free electrocatalyst for hydrogen evolution reaction and semicarbazide oxidation
Studies of metal-free carbon nanostructures prove effective in energy and environmental applications due to their molecular tunability and vast chemical space. Herein, we synthesize nitrogen-containing multi-walled carbon nanotubes (N-MWCNTs) via. acid-catalysed incorporation of 3, 4-diaminopyridine into multi-walled carbon nanotubes (MWCNTs), and demonstrating their efficacy in electrocatalytic hydrogen evolution reaction (HER) and semicarbazide (SCB) oxidation for energy and environmental waste management, respectively. Successful synthesis is further confirmed by analysis techniques, i.e. Fourier transform infrared (FTIR) spectral analysis shows the diminishing OH frequency around 3250 cm−1 in MWCNTs after functionalization and the formation of an OC–NH bond in N-MWCNTs at 1710 cm−1. X-ray diffraction (XRD) confirms the incorporation of N-species, while Raman spectroscopic analysis indicates an increase in the ID/IG ratio MWCNTs (∼1) to N-MWCNTs (∼1.25), suggesting more defective sites in the N-MWCNTs nanocomposite. X-ray photoelectron spectroscopy (XPS) reveals peaks at 399.38, 400.49, and 402.05 eV, attributed to pyridinic-N, aromatic amide-N, and protonated amine groups, respectively. N₂ adsorption-desorption studies shows a high Brunauer-Emmett-Teller (BET) surface area for N-MWCNTs (119.22 m2/g) compared to MWCNTs (74.94 m2/g). Linear sweep voltammetry (LSV) profiles demonstrate enhanced activity of N-MWCNTs for both HER and SCB oxidation at an ultralow potential of E = −0.55 V vs RHE at 10 mA/cm2, with a lower Tafel slope of 108 mV.dec−1. Moreover, the electrochemical sensing studies indicates on N-MWCNTs were demonstrating an efficient electron transfer to SCB with the lower detection limit of 0.004 μmol. This work provides carbon-based metal-free electrocatalysts for energy harvesting and environmental management.
期刊介绍:
The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc.
The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.