Technical note: Intercomparison Study of the EC Radiocarbon Analysis Methods Using Synthetic Known Samples

Zhang, Xiangyun; Li, Jun; Zhu, Sanyuan; Liu, Junwen; Ding, Ping; Gao, Shutao; Tian, Chongguo; Chen, Yingjun; Peng, Ping'an; Zhang, Gan

doi:https://doi.org/10.5194/egusphere-2023-379

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https://doi.org/10.5194/egusphere-2023-379

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28 Mar 2023

| 28 Mar 2023

Technical note: Intercomparison Study of the EC Radiocarbon Analysis Methods Using Synthetic Known Samples

Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang

Abstract. The accurate identification of elemental carbon (EC) source in aerosol based on radiocarbon (¹⁴C) depends on the method of EC isolation. The lack of aerosol EC reference materials with "true" ¹⁴C values makes it impossible to evaluate the accuracy of various methods for the analysis of ¹⁴C-EC in aerosols. In this study, EC separation methods were evaluated by using samples of mixed biomass burning, vehicle exhaust and coal-combustion. The results show that ¹⁴C-EC was not only related to the separation method but also to the types and proportions of biomass sources in the sample. And the Hydropyrolysis (Hypy) method, which can be used to separate a highly stable portion of EC_Hypy and avoid charring, is a more effective and stable approach for the matrix-independent ¹⁴C quantification of EC in aerosols. The ¹³C-EC_Hypy and non-fossil EC_Hypy values of SRM1649b was 24.9 ‰ and 11 %, respectively.

Received: 03 Mar 2023 – Discussion started: 28 Mar 2023

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Journal article(s) based on this preprint

11 Jul 2023

Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples

Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang

Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023,https://doi.org/10.5194/acp-23-7495-2023, 2023

Short summary

Xiangyun Zhang et al.

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-379', Anonymous Referee #1, 14 Apr 2023

This paper uses a set of synthetic black carbon-containing aerosol mixtures made from materials with known composition to assess the ability of four different techniues used to isolate the black carbon component for carbon isotope determination (13C and 14C). The advantage of this approach is that the 'true' results are known, and thereofre the reliability of th methods used can be assessed. This is an innovative approach to the long-standing issues around method specific analytical biases, and therefore I think represents a signficant step forward in achiveing more reliable source apportionment for aerosol samples. This is important because of the significant role that black carbon in aerosols plays in anthropogenic warming. The study fingd that the hypy technique out-performs the other techniques in its ability to produce reliable results across a range of BC compositions.
I think the paper is well and clearly written and the experimental and analytical components sound. I have no substantive issues with the interpretaion or conclusions of the study, but have made a number of grammatical suggestions, with some requests for clarification on the annotated pdf attached.

Citation: https://doi.org/10.5194/egusphere-2023-379-RC1
- AC1: 'Reply on RC1', Xiangyun Zhang, 20 May 2023
  
  We thank the reviewer for careful reading and valuable comments.You can find a detailed response to the reviewer’s comments on the attached supplement.
  
  Citation: https://doi.org/10.5194/egusphere-2023-379-AC1
RC2:
'Comment on egusphere-2023-379', Will Meredith, 18 Apr 2023

This short paper by Zhang et al is a nice attempt to explore some of the difficulties of quantifying and especially isotopically characterisation the “black carbon” fraction of a number of reference materials. Full disclosure – as one of the people responsible for developing the HyPy methodology I was delighted to see it applied here, and that it performed quite well against some of the other techniques.
That said my main comment on the paper is that the authors need to get to grips with te terminology used. They appear to use BC and EC interchangeably throughout and also OC and TC. I’m not sure TC is actually defined anywhere either. In both cases it would probably be better if you were consistent with terminology used throughout so that the reader is not confused. Generally I think I know what you intend, but it is not clear. As an example in line 210 you use both EC continuum and BC continuum in the same sentence. Likewise you talk about “separating” EC from OC, but they are part of the same thing so “isolating” may be better.

More minor comments. Don’t use initials in citations in the text (e.g. line 76, 80, 97 and others). Do use dates in the list (unless not to is a weird requirement of the journal).
Line 197 – sentence beginning “Compared with” currently does not make sense.
Line 202 – “Black carbon isotopes” specifically or black carbon content?
Line 282 – “coking” should this read “charring”?
NMR and SEM are brought into the discussion but not previously introduced into the methods section.

Citation: https://doi.org/10.5194/egusphere-2023-379-RC2
- AC2: 'Reply on RC2', Xiangyun Zhang, 20 May 2023
  
  We thank the reviewer for careful reading and valuable comments.You can find a detailed response to the reviewer’s comments on the attached supplement.
  
  Citation: https://doi.org/10.5194/egusphere-2023-379-AC2

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-379', Anonymous Referee #1, 14 Apr 2023

This paper uses a set of synthetic black carbon-containing aerosol mixtures made from materials with known composition to assess the ability of four different techniues used to isolate the black carbon component for carbon isotope determination (13C and 14C). The advantage of this approach is that the 'true' results are known, and thereofre the reliability of th methods used can be assessed. This is an innovative approach to the long-standing issues around method specific analytical biases, and therefore I think represents a signficant step forward in achiveing more reliable source apportionment for aerosol samples. This is important because of the significant role that black carbon in aerosols plays in anthropogenic warming. The study fingd that the hypy technique out-performs the other techniques in its ability to produce reliable results across a range of BC compositions.
I think the paper is well and clearly written and the experimental and analytical components sound. I have no substantive issues with the interpretaion or conclusions of the study, but have made a number of grammatical suggestions, with some requests for clarification on the annotated pdf attached.

Citation: https://doi.org/10.5194/egusphere-2023-379-RC1
- AC1: 'Reply on RC1', Xiangyun Zhang, 20 May 2023
  
  We thank the reviewer for careful reading and valuable comments.You can find a detailed response to the reviewer’s comments on the attached supplement.
  
  Citation: https://doi.org/10.5194/egusphere-2023-379-AC1
RC2:
'Comment on egusphere-2023-379', Will Meredith, 18 Apr 2023

This short paper by Zhang et al is a nice attempt to explore some of the difficulties of quantifying and especially isotopically characterisation the “black carbon” fraction of a number of reference materials. Full disclosure – as one of the people responsible for developing the HyPy methodology I was delighted to see it applied here, and that it performed quite well against some of the other techniques.
That said my main comment on the paper is that the authors need to get to grips with te terminology used. They appear to use BC and EC interchangeably throughout and also OC and TC. I’m not sure TC is actually defined anywhere either. In both cases it would probably be better if you were consistent with terminology used throughout so that the reader is not confused. Generally I think I know what you intend, but it is not clear. As an example in line 210 you use both EC continuum and BC continuum in the same sentence. Likewise you talk about “separating” EC from OC, but they are part of the same thing so “isolating” may be better.

More minor comments. Don’t use initials in citations in the text (e.g. line 76, 80, 97 and others). Do use dates in the list (unless not to is a weird requirement of the journal).
Line 197 – sentence beginning “Compared with” currently does not make sense.
Line 202 – “Black carbon isotopes” specifically or black carbon content?
Line 282 – “coking” should this read “charring”?
NMR and SEM are brought into the discussion but not previously introduced into the methods section.

Citation: https://doi.org/10.5194/egusphere-2023-379-RC2
- AC2: 'Reply on RC2', Xiangyun Zhang, 20 May 2023
  
  We thank the reviewer for careful reading and valuable comments.You can find a detailed response to the reviewer’s comments on the attached supplement.
  
  Citation: https://doi.org/10.5194/egusphere-2023-379-AC2

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload

AR by Xiangyun Zhang on behalf of the Authors (20 May 2023) Author's response Author's tracked changes Manuscript

ED: Publish as is (05 Jun 2023) by Katye Altieri

AR by Xiangyun Zhang on behalf of the Authors (07 Jun 2023) Manuscript

Journal article(s) based on this preprint

11 Jul 2023

Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples

Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang

Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023,https://doi.org/10.5194/acp-23-7495-2023, 2023

Short summary

Xiangyun Zhang et al.

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https://doi.org/10.5194/egusphere-2023-379-supplement

Xiangyun Zhang et al.

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The results show that ¹⁴C-EC was not only related to the separation method but also to the types and proportions of biomass sources in the sample. According to the ratio 58 : 42 of crop residue burning and firewood combustion on average worldly, the non-fossil EC value of aerosol obtained by the Hypy method is closest to the theoretical value. And the ¹³C-EC_Hypy and non-fossil EC_Hypy values of SRM1649b was 24.9 ‰ and 11 %, respectively.


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