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A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes

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A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes. / Wan, Zhonghao; Sun, Yuqing; Tsang, Daniel C.W.; Yu, Iris K.M.; Fan, Jiajun; Clark, James H.; Zhou, Yaoyu; Cao, Xinde; Gao, Bin; Ok, Yong Sik.

In: Green Chemistry, Vol. 21, No. 17, 18.08.2019, p. 4800-4814.

Research output: Contribution to journalArticlepeer-review

Harvard

Wan, Z, Sun, Y, Tsang, DCW, Yu, IKM, Fan, J, Clark, JH, Zhou, Y, Cao, X, Gao, B & Ok, YS 2019, 'A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes', Green Chemistry, vol. 21, no. 17, pp. 4800-4814. https://doi.org/10.1039/c9gc01843c

APA

Wan, Z., Sun, Y., Tsang, D. C. W., Yu, I. K. M., Fan, J., Clark, J. H., Zhou, Y., Cao, X., Gao, B., & Ok, Y. S. (2019). A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes. Green Chemistry, 21(17), 4800-4814. https://doi.org/10.1039/c9gc01843c

Vancouver

Wan Z, Sun Y, Tsang DCW, Yu IKM, Fan J, Clark JH et al. A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes. Green Chemistry. 2019 Aug 18;21(17):4800-4814. https://doi.org/10.1039/c9gc01843c

Author

Wan, Zhonghao ; Sun, Yuqing ; Tsang, Daniel C.W. ; Yu, Iris K.M. ; Fan, Jiajun ; Clark, James H. ; Zhou, Yaoyu ; Cao, Xinde ; Gao, Bin ; Ok, Yong Sik. / A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes. In: Green Chemistry. 2019 ; Vol. 21, No. 17. pp. 4800-4814.

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@article{8c151b129d444fcdb685c9f091786fff,
title = "A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes",
abstract = "We have developed a wood waste-derived biochar as a sustainable graphitic carbon catalyst for environmental remediation through catalytic pyrolysis under the synergistic effects between Cu heteroatoms and CO2, which for the first time are found to significantly enhance the oxygen functionalities, defective sites, and highly ordered sp2-hybridized carbon matrix. The copper-doped graphitic biochars (Cu-GBCs) were further characterized by XRD, FTIR, Raman, XPS, etc., revealing that the modified specific surface area, pore structure, graphitization, and active sites (i.e., defective sites and ketonic group) on the Cu-GBCs corresponded to the synergistic Cu species loading and Cu-induced carbon-matrix reformation in CO2 environment during pyrolysis. The catalytic ability of Cu-GBCs was evaluated using the ubiquitous peroxydisulfate (PDS) activation system for the removal of various organic contaminants (i.e., rhodamine B, phenol, bisphenol A, and 4-chlorophenol), and gave the highest degradation rate of 0.0312 min-1 in comparison with those of pristine GBCs and N2-pyrolyzed Cu-GBCs ranging from 0.0056 to 0.0094 min-1. The synergistic effects were attributed to the encapsulated Cu heteroatoms, evolved ketonic groups, and abundant unconfined π electrons within the carbon lattice. According to scavenger experiments, ESR analysis, and two-chamber experiments, selective and sustainable non-radical pathways (i.e., singlet oxygenation and electron transfer) mediated by the Cu-induced metastable surface complex were achieved in the Cu-GBC/PDS system. This study offers the first insights into the efficacy, sustainability, and mechanistic roles of Cu-GBCs as an emerging carbon-based catalyst for green environmental remediation.",
author = "Zhonghao Wan and Yuqing Sun and Tsang, {Daniel C.W.} and Yu, {Iris K.M.} and Jiajun Fan and Clark, {James H.} and Yaoyu Zhou and Xinde Cao and Bin Gao and Ok, {Yong Sik}",
note = "{\textcopyright} The Royal Society of Chemistry 2019. This is an author-produced version of the published paper. Uploaded in accordance with the publisher{\textquoteright}s self-archiving policy. Further copying may not be permitted; contact the publisher for details. ",
year = "2019",
month = aug,
day = "18",
doi = "10.1039/c9gc01843c",
language = "English",
volume = "21",
pages = "4800--4814",
journal = "Green Chemistry",
issn = "1463-9270",
publisher = "Royal Society of Chemistry",
number = "17",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - A sustainable biochar catalyst synergized with copper heteroatoms and CO2 for singlet oxygenation and electron transfer routes

AU - Wan, Zhonghao

AU - Sun, Yuqing

AU - Tsang, Daniel C.W.

AU - Yu, Iris K.M.

AU - Fan, Jiajun

AU - Clark, James H.

AU - Zhou, Yaoyu

AU - Cao, Xinde

AU - Gao, Bin

AU - Ok, Yong Sik

N1 - © The Royal Society of Chemistry 2019. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

PY - 2019/8/18

Y1 - 2019/8/18

N2 - We have developed a wood waste-derived biochar as a sustainable graphitic carbon catalyst for environmental remediation through catalytic pyrolysis under the synergistic effects between Cu heteroatoms and CO2, which for the first time are found to significantly enhance the oxygen functionalities, defective sites, and highly ordered sp2-hybridized carbon matrix. The copper-doped graphitic biochars (Cu-GBCs) were further characterized by XRD, FTIR, Raman, XPS, etc., revealing that the modified specific surface area, pore structure, graphitization, and active sites (i.e., defective sites and ketonic group) on the Cu-GBCs corresponded to the synergistic Cu species loading and Cu-induced carbon-matrix reformation in CO2 environment during pyrolysis. The catalytic ability of Cu-GBCs was evaluated using the ubiquitous peroxydisulfate (PDS) activation system for the removal of various organic contaminants (i.e., rhodamine B, phenol, bisphenol A, and 4-chlorophenol), and gave the highest degradation rate of 0.0312 min-1 in comparison with those of pristine GBCs and N2-pyrolyzed Cu-GBCs ranging from 0.0056 to 0.0094 min-1. The synergistic effects were attributed to the encapsulated Cu heteroatoms, evolved ketonic groups, and abundant unconfined π electrons within the carbon lattice. According to scavenger experiments, ESR analysis, and two-chamber experiments, selective and sustainable non-radical pathways (i.e., singlet oxygenation and electron transfer) mediated by the Cu-induced metastable surface complex were achieved in the Cu-GBC/PDS system. This study offers the first insights into the efficacy, sustainability, and mechanistic roles of Cu-GBCs as an emerging carbon-based catalyst for green environmental remediation.

AB - We have developed a wood waste-derived biochar as a sustainable graphitic carbon catalyst for environmental remediation through catalytic pyrolysis under the synergistic effects between Cu heteroatoms and CO2, which for the first time are found to significantly enhance the oxygen functionalities, defective sites, and highly ordered sp2-hybridized carbon matrix. The copper-doped graphitic biochars (Cu-GBCs) were further characterized by XRD, FTIR, Raman, XPS, etc., revealing that the modified specific surface area, pore structure, graphitization, and active sites (i.e., defective sites and ketonic group) on the Cu-GBCs corresponded to the synergistic Cu species loading and Cu-induced carbon-matrix reformation in CO2 environment during pyrolysis. The catalytic ability of Cu-GBCs was evaluated using the ubiquitous peroxydisulfate (PDS) activation system for the removal of various organic contaminants (i.e., rhodamine B, phenol, bisphenol A, and 4-chlorophenol), and gave the highest degradation rate of 0.0312 min-1 in comparison with those of pristine GBCs and N2-pyrolyzed Cu-GBCs ranging from 0.0056 to 0.0094 min-1. The synergistic effects were attributed to the encapsulated Cu heteroatoms, evolved ketonic groups, and abundant unconfined π electrons within the carbon lattice. According to scavenger experiments, ESR analysis, and two-chamber experiments, selective and sustainable non-radical pathways (i.e., singlet oxygenation and electron transfer) mediated by the Cu-induced metastable surface complex were achieved in the Cu-GBC/PDS system. This study offers the first insights into the efficacy, sustainability, and mechanistic roles of Cu-GBCs as an emerging carbon-based catalyst for green environmental remediation.

UR - http://www.scopus.com/inward/record.url?scp=85071250205&partnerID=8YFLogxK

U2 - 10.1039/c9gc01843c

DO - 10.1039/c9gc01843c

M3 - Article

AN - SCOPUS:85071250205

VL - 21

SP - 4800

EP - 4814

JO - Green Chemistry

JF - Green Chemistry

SN - 1463-9270

IS - 17

ER -