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Metal-Free Carbocatalysis in Advanced Oxidation Reactions
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Conspectus Catalytic processes have remarkably boosted the rapid industrializations in chemical production, energy conversion, and environmental remediation. As one of the emerging applications of carbocatalysis, metal-free nanocarbons have demonstrated promise as catalysts for green remediation technologies to overcome the poor stability and undesirable metal leaching in metal-based advanced oxidation processes (AOPs). Since our reports of heterogeneous activation of persulfates with low-dimensional nanocarbons, the novel oxidative system has raised tremendous interest for degradation of organic contaminants in wastewater without secondary contamination. In this Account, we showcase our recent contributions to metal-free catalysis in advanced oxidation, including design of nanocarbon catalysts, exploration of intrinsic active sites, and identification of reactive species and reaction pathways, and we offer perspectives on carbocatalysis for future environmental applications. The journey starts with the discovery of peroxymonosulfate (PMS) and peroxydisulfate (PDS) activation by graphene-based materials. With the systematic investigations on most carbon allotropes, for the first time the carbocatalysis for PMS or PDS activation was correlated with the pristine carbon configuration, oxygen functionality (ketonic groups), defect degree (exposed edge sites and vacancies), and dimensional structure. Moreover, an intrinsic difference in catalytic oxidation does exist between PMS and PDS activation. For example, the PMS/carbon reaction is dominated by free radicals, while PDS/carbon catalysis was unveiled as a singlet oxygen- or nonradical-based process in which the surface-activated PDS complex directly degrades the organic pollutants without relying on the generation of free radicals. Nitrogen doping significantly enhances the carbocatalysis because of the positively charged carbon domains, which strongly bind with persulfates to form reactive intermediates toward organic reactions. More importantly, N doping substantially alters the catalytic oxidation from a radical process to a nonradical pathway in PMS activation. Codoping of sulfur or boron with nitrogen at a rational level will synergistically promote the catalysis as a result of the formation of more catalytic centers by improved charge/spin redistribution of the carbon framework. Furthermore, a structure–performance relationship was established for annealed nanodiamonds with a characteristic sp 3 /sp 2 (core/shell) hybridization, where the catalytic pathways were intimately dependent on the thickness of the graphitic shells. Interestingly, the introduction of structural defects and N dopants into the well-defined graphitic carbon framework and alteration of graphene/diamond hybrids can transform the persulfate/carbon system from a radical oxidation pathway to a nonradical pathway. Encapsulation of metal nanoparticles within carbon layers further modulates the electronic states of the interacting carbon via charge transport to increase the electron density. Overall, this Account contributes to unveiling the mist of carbocatalysis in AOPs and to summarizing the achievements of metal-free remediation. We also present future research directions on underpinning the knowledge base to facilitate the applications of nanocarbons in sustainable catalysis and environmental chemistry.
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Cites
Oh, W., Dong, Z., & Lim, T. (2016) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2016.04.003 · Cited by 2,609
Liang, J., Jiao, Y., Jaroniec, M., & Qiao, S. (2012) · Angewandte Chemie International Edition · doi:10.1002/anie.201206720 · Cited by 2,105
Environmental Applications of Carbon-Based Nanomaterials
Mauter, M. S., & Elimelech, M. (2008) · Environmental Science & Technology · doi:10.1021/es8006904 · Cited by 1,587
Nanocarbons for the Development of Advanced Catalysts
Su, D. S., Perathoner, S., & Centi, G. (2013) · Chemical Reviews · doi:10.1021/cr300367d · Cited by 1,341
Iron Encapsulated within Pod‐like Carbon Nanotubes for Oxygen Reduction Reaction
Deng, D., Yu, L., Chen, X., Wang, G., Li, J., Pan, X., Deng, J., Sun, G., & Bao, X. (2012) · Angewandte Chemie International Edition · doi:10.1002/anie.201204958 · Cited by 1,319
Activation of Peroxymonosulfate by Benzoquinone: A Novel Nonradical Oxidation Process
Zhou, Y., Jiang, J., Gao, Y., Ma, J., Pang, S., Li, J., Lu, X., & Yuan, L.-P. (2015) · Environmental Science & Technology · doi:10.1021/acs.est.5b03595 · Cited by 1,279
Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes
Cheng, X., Guo, H., Zhang, Y., Wu, X. Z., & Liu, Y. (2017) · Water Research · doi:10.1016/j.watres.2017.02.016 · Cited by 1,062
Two‐Step Boron and Nitrogen Doping in Graphene for Enhanced Synergistic Catalysis
Zheng, Y., Jiao, Y., Ge, L., Jaroniec, M., & Qiao, S. (2013) · Angewandte Chemie International Edition · doi:10.1002/anie.201209548 · Cited by 1,051
Duan, X., Sun, H., Wang, Y., Kang, J., & Wang, S. (2014) · ACS Catalysis · doi:10.1021/cs5017613 · Cited by 940
Self-citationInsights into Heterogeneous Catalysis of Persulfate Activation on Dimensional-Structured Nanocarbons
Duan, X., Sun, H., Kang, J., Wang, Y., Indrawirawan, S., & Wang, S. (2015) · ACS Catalysis · doi:10.1021/acscatal.5b00774 · Cited by 799
Self-citationZhang, T., Chen, Y., Wang, Y., Le Roux, J., Yang, Y., & Croué, J.-P. (2014) · Environmental Science & Technology · doi:10.1021/es501218f · Cited by 798
Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis
Duan, X., Ao, Z., Sun, H., Indrawirawan, S., Wang, Y., Kang, J., Liang, F., Zhu, Z., & Wang, S. (2015) · ACS Applied Materials & Interfaces · doi:10.1021/am508416n · Cited by 781
Self-citationDuan, X., Ao, Z., Zhou, L., Sun, H., Wang, G., & Wang, S. (2016) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2016.01.059 · Cited by 732
Self-citationReduced Graphene Oxide for Catalytic Oxidation of Aqueous Organic Pollutants
Sun, H., Liu, S., Zhou, G., Ang, H. M., Tadé, M. O., & Wang, S. (2012) · ACS Applied Materials & Interfaces · doi:10.1021/am301372d · Cited by 722
Self-citationHu, P., Su, H., Chen, Z., Yu, C., Li, Q., Zhou, B., Alvarez, P. J. J., & Long, M. (2017) · Environmental Science & Technology · doi:10.1021/acs.est.7b03014 · Cited by 706
Sulfur and Nitrogen Co-Doped Graphene for Metal-Free Catalytic Oxidation Reactions
Duan, X., O'Donnell, K. M., Sun, H., Wang, Y., & Wang, S. (2015) · Small · doi:10.1002/smll.201403715 · Cited by 703
Self-citationShao, P., Tian, J., Yang, F., Duan, X., Gao, S., Shi, W., Luo, X., Cui, F., Luo, S., & Wang, S. (2018) · Advanced Functional Materials · doi:10.1002/adfm.201705295 · Cited by 696
Self-citationActivation of Persulfates by Graphitized Nanodiamonds for Removal of Organic Compounds
Lee, H., Kim, H.-I., Weon, S., Choi, W., Hwang, Y. S., Seo, J., Lee, C., & Kim, J.-H. (2016) · Environmental Science & Technology · doi:10.1021/acs.est.6b02079 · Cited by 688
Lee, H., Lee, H.-J., Jeong, J., Lee, J., Park, N.-B., & Lee, C. (2014) · Chemical Engineering Journal · doi:10.1016/j.cej.2014.12.065 · Cited by 674
Wang, X., Qin, Y., Zhu, L., & Tang, H. (2015) · Environmental Science & Technology · doi:10.1021/acs.est.5b01059 · Cited by 674
Carbocatalysts: Graphene Oxide and Its Derivatives
Su, C., & Loh, K. P. (2012) · Accounts of Chemical Research · doi:10.1021/ar300118v · Cited by 574
Sun, H., Kwan, C., Suvorova, A., Ang, H. M., Tadé, M. O., & Wang, S. (2014) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2014.02.012 · Cited by 509
Self-citationUnveiling the active sites of graphene-catalyzed peroxymonosulfate activation
Duan, X., Sun, H., Ao, Z., Zhou, L., Wang, G., & Wang, S. (2016) · Carbon · doi:10.1016/j.carbon.2016.06.016 · Cited by 498
Self-citationSurface controlled generation of reactive radicals from persulfate by carbocatalysis on nanodiamonds
Duan, X., Su, C., Zhou, L., Sun, H., Suvorova, A. A., Odedairo, T., Zhu, Z., Shao, Z., & Wang, S. (2016) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2016.04.043 · Cited by 489
Self-citationUnique chemical reactivity of a graphene nanoribbon’s zigzag edge
Jiang, D., Sumpter, B. G., & Dai, S. (2007) · The Journal of Chemical Physics · doi:10.1063/1.2715558 · Cited by 476
Liang, P., Zhang, C., Duan, X., Sun, H., Liu, S., Tadé, M. O., & Wang, S. (2017) · Environmental Science Nano · doi:10.1039/c6en00633g · Cited by 467
Self-citationYao, Y., Chen, H., Lian, C., Wei, F., Zhang, D., Wu, G., Chen, B., & Wang, S. (2016) · Journal of Hazardous Materials · doi:10.1016/j.jhazmat.2016.03.089 · Cited by 442
Self-citationRecent Progress on the Growth Mechanism of Carbon Nanotubes: A Review
Tessonnier, J., & Su, D. S. (2011) · ChemSusChem · doi:10.1002/cssc.201100175 · Cited by 427
Li, D., Duan, X., Sun, H., Kang, J., Zhang, H., Tadé, M. O., & Wang, S. (2017) · Carbon · doi:10.1016/j.carbon.2017.01.058 · Cited by 396
Self-citationYun, E.-T., Yoo, H.-Y., Bae, H., Kim, H., & Lee, J. (2017) · Environmental Science & Technology · doi:10.1021/acs.est.7b02519 · Cited by 360
Zhou, Y., Jiang, J., Gao, Y., Pang, S., Yang, Y., Ma, J., Gu, J., Li, J., Wang, Z., Wang, L.-H., et al. (2017) · Water Research · doi:10.1016/j.watres.2017.08.049 · Cited by 348
Wang, Y., Ao, Z., Sun, H., Duan, X., & Wang, S. (2016) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2016.05.075 · Cited by 345
Self-citationSun, H., Wang, Y., Liu, S., Ge, L., Wang, L., Zhu, Z., & Wang, S. (2013) · Chemical Communications · doi:10.1039/c3cc43401j · Cited by 336
Self-citationYao, Y., Chen, H., Qin, J., Wu, G., Lian, C., Zhang, J., & Wang, S. (2016) · Water Research · doi:10.1016/j.watres.2016.05.065 · Cited by 332
Self-citationMass production and industrial applications of graphene materials
Zhu, Y., Ji, H., Cheng, H., & Ruoff, R. S. (2017) · National Science Review · doi:10.1093/nsr/nwx055 · Cited by 319
Indrawirawan, S., Sun, H., Duan, X., & Wang, S. (2015) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2015.05.049 · Cited by 318
Self-citationDuan, X., Ao, Z., Sun, H., Zhou, L., Wang, G., & Wang, S. (2015) · Chemical Communications · doi:10.1039/c5cc05101k · Cited by 316
Self-citationLi, X., Ao, Z., Liu, J., Sun, H., Rykov, A. I., & Wang, J. (2016) · ACS Nano · doi:10.1021/acsnano.6b07522 · Cited by 306
Self-citationDuan, X., Ao, Z., Zhang, H., Saunders, M., Sun, H., Shao, Z., & Wang, S. (2017) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2017.10.007 · Cited by 298
Self-citationLiang, P., Zhang, C., Duan, X., Sun, H., Liu, S., Tadé, M. O., & Wang, S. (2017) · ACS Sustainable Chemistry & Engineering · doi:10.1021/acssuschemeng.6b03035 · Cited by 289
Self-citationWang, Y., Sun, H., Duan, X., Ang, H. M., Tadé, M. O., & Wang, S. (2015) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2015.02.016 · Cited by 283
Self-citationTian, W., Zhang, H., Duan, X., Sun, H., Tade, M. O., Ang, H. M., & Wang, S. (2016) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.6b01748 · Cited by 259
Self-citationCarbocatalysis in Liquid‐Phase Reactions
Su, D. S., Wen, G., Wu, S., Peng, F., & Schlögl, R. (2016) · Angewandte Chemie International Edition · doi:10.1002/anie.201600906 · Cited by 254
Kang, J., Duan, X., Wang, C., Sun, H., Tan, X., Tadé, M. O., & Wang, S. (2017) · Chemical Engineering Journal · doi:10.1016/j.cej.2017.09.102 · Cited by 235
Self-citationLow temperature combustion synthesis of nitrogen-doped graphene for metal-free catalytic oxidation
Indrawirawan, S., Sun, H., Duan, X., & Wang, S. (2014) · Journal of Materials Chemistry A · doi:10.1039/c4ta05940a · Cited by 226
Self-citationEffects of nitrogen-, boron-, and phosphorus-doping or codoping on metal-free graphene catalysis
Duan, X., Indrawirawan, S., Sun, H., & Wang, S. (2014) · Catalysis Today · doi:10.1016/j.cattod.2014.10.005 · Cited by 213
Self-citationWang, C., Kang, J., Liang, P., Zhang, H., Sun, H., Tadé, M. O., & Wang, S. (2016) · Environmental Science Nano · doi:10.1039/c6en00397d · Cited by 213
Self-citationPeng, W., Liu, S., Sun, H., Yao, Y., Zhi, L., & Wang, S. (2013) · Journal of Materials Chemistry A · doi:10.1039/c3ta10592j · Cited by 209
Self-citationSurface-tailored nanodiamonds as excellent metal-free catalysts for organic oxidation
Duan, X., Ao, Z., Li, D., Sun, H., Zhou, L., Suvorova, A. A., Saunders, M., Wang, G., & Wang, S. (2016) · Carbon · doi:10.1016/j.carbon.2016.03.034 · Cited by 202
Self-citationCarbocatalytic activation of persulfate for removal of antibiotics in water solutions
Kang, J., Duan, X., Zhou, L., Sun, H., Tadé, M. O., & Wang, S. (2015) · Chemical Engineering Journal · doi:10.1016/j.cej.2015.12.040 · Cited by 201
Self-citationYao, Y., Lian, C., Wu, G., Hu, Y., Wei, F., Yu, M., & Wang, S. (2017) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2017.07.064 · Cited by 175
Self-citationOne-pot synthesis of N-doped graphene for metal-free advanced oxidation processes
Wang, C., Kang, J., Sun, H., Ang, H. M., Tadé, M. O., & Wang, S. (2016) · Carbon · doi:10.1016/j.carbon.2016.02.048 · Cited by 170
Self-citationLiu, S., Peng, W., Sun, H., & Wang, S. (2013) · Nanoscale · doi:10.1039/c3nr04282k · Cited by 164
Self-citationChen, H., & Carroll, K. C. (2016) · Environmental Pollution · doi:10.1016/j.envpol.2016.04.088 · Cited by 141
Kim, H., Bak, S., Lee, S. W., Kim, M.-S., Park, B., Lee, S. C., Choi, Y. J., Jun, S. C., Han, J. T., Nam, K., et al. (2016) · Energy & Environmental Science · doi:10.1039/c5ee03580e · Cited by 138
Tian, W., Zhang, H., Sun, H., Tadé, M. O., & Wang, S. (2017) · Carbon · doi:10.1016/j.carbon.2017.03.027 · Cited by 109
Self-citationComment on “Activation of Persulfate by Graphitized Nanodiamonds for Removal of Organic Compounds”
Duan, X., Sun, H., & Wang, S. (2017) · Environmental Science & Technology · doi:10.1021/acs.est.7b00399 · Cited by 19
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Metadata
- Authors
- Duan, X., Sun, H., & Wang, S.
- Affiliations
- Curtin University (AU)
- Edith Cowan University (AU)
- Corresponding author
- Sun, Hongqi
- Wang, Shaobin
- Venue
- Accounts of Chemical Research
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-03-01
- Volume
- 51
- Issue
- 3
- Pages
- 678-687
- ISSN
- 0001-4842 (ISSN-L)
- 1520-4898
- OpenAlex
- W2790656902
- Cited by
- 1,329
- References
- 57
- Citations by year
- 2026: 84 · 2025: 148 · 2024: 163 · 2023: 205 · 2022: 242 · 2021: 180 · 2020: 138 · 2019: 130 · 2018: 39
- FWCI
- 53.38
- Type
- journal article
- Language
- en
- Open access
- green
- ro.ecu.edu.au
- Locations
- Accounts of Chemical Research (publishedVersion)
- PubMed (publishedVersion)
- Australasian Journal of Paramedicine (submittedVersion)
- Adelaide Research & Scholarship (AR&S) (University of Adelaide) (submittedVersion)
- eSpace (Curtin University) (submittedVersion)
- Funders
- Australian Research Council (DP150103026)
- Topics
- Physical Sciences › Environmental Science › Water Science and Technology › Advanced oxidation water treatment
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Physical Sciences › Environmental Science › Environmental Engineering › Environmental remediation with nanomaterials
- Keywords
- carbocatalysis, metal-free catalysts, advanced oxidation processes, persulfate activation, carbon nanomaterials, graphene, nitrogen-doped carbon, nanodiamonds, graphitic carbon, reactive oxygen species, singlet oxygen, free radicals, organic pollutant degradation, wastewater remediation, structure-performance relationship
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