Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction
Photoreforming lignocellulose into valuable fuels and chemicals represents an environmentally friendly and energy-saving technology. Herein, a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction (Fe-SA/PCN-HJ) is constructed for highly efficient photocatalytic reforming of...
| Main Authors: | , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2025
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| Online Access: | https://hdl.handle.net/10356/182089 |
| _version_ | 1826109875194691584 |
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| author | Chen, Yanglin Zheng, Mei Sun, Jiajun Xu, Jianzhong Wu, Chao Liu, Jiyuan He, Limo Xi, Shibo Li, Shuzhou Xue, Can |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Chen, Yanglin Zheng, Mei Sun, Jiajun Xu, Jianzhong Wu, Chao Liu, Jiyuan He, Limo Xi, Shibo Li, Shuzhou Xue, Can |
| author_sort | Chen, Yanglin |
| collection | NTU |
| description | Photoreforming lignocellulose into valuable fuels and chemicals represents an environmentally friendly and energy-saving technology. Herein, a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction (Fe-SA/PCN-HJ) is constructed for highly efficient photocatalytic reforming of lignocellulose into CO and lactic acid, wherein Fe single atoms are confined to the surface of the PCN-HJ. Experimental investigations and density functional theory (DFT) calculations reveal that the homojunctions and dispersed Fe atoms on the surface greatly improve the separation efficiency and transport of photogenerated charge carriers. As such, driven by the internal electric field across the entire junction, the photoinduced electrons can rapidly migrate from the bulk to the surface, leading to the enrichment of surface electrons at the dispersed Fe-N4 sites. In addition, the Fe-N4 sites optimize the adsorption and activation of molecular oxygen and facilitate electron transfer to the adsorbed molecular oxygen, thereby promoting the formation of reactive oxygen species for lignocellulose photoreforming. Under full spectrum irradiation for 2 h, the Fe-SA/PCN-HJ exhibits an ultrahigh CO generation rate of 92.33 mmol g-1 and yields 136.21 mg of lactic acid by using 900 mg of fructose as the model substrate. Moreover, we have further demonstrated that the Fe-SA/PCN-HJ photocatalyst presents universally applicable capabilities for the photoreforming of various types of lignocellulosic biomass. This work provides an approach for the production of CO and lactic acid through the photoreforming of lignocellulose, which is promising for the production of fuels and valuable chemicals. |
| first_indexed | 2025-03-09T09:54:46Z |
| format | Journal Article |
| id | ntu-10356/182089 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-03-09T09:54:46Z |
| publishDate | 2025 |
| record_format | dspace |
| spelling | ntu-10356/1820892025-01-10T15:50:21Z Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction Chen, Yanglin Zheng, Mei Sun, Jiajun Xu, Jianzhong Wu, Chao Liu, Jiyuan He, Limo Xi, Shibo Li, Shuzhou Xue, Can School of Materials Science and Engineering School of Chemistry, Chemical Engineering and Biotechnology Chemistry Photoreforming of lignocellulose CO and lactic acid coproduction Photoreforming lignocellulose into valuable fuels and chemicals represents an environmentally friendly and energy-saving technology. Herein, a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction (Fe-SA/PCN-HJ) is constructed for highly efficient photocatalytic reforming of lignocellulose into CO and lactic acid, wherein Fe single atoms are confined to the surface of the PCN-HJ. Experimental investigations and density functional theory (DFT) calculations reveal that the homojunctions and dispersed Fe atoms on the surface greatly improve the separation efficiency and transport of photogenerated charge carriers. As such, driven by the internal electric field across the entire junction, the photoinduced electrons can rapidly migrate from the bulk to the surface, leading to the enrichment of surface electrons at the dispersed Fe-N4 sites. In addition, the Fe-N4 sites optimize the adsorption and activation of molecular oxygen and facilitate electron transfer to the adsorbed molecular oxygen, thereby promoting the formation of reactive oxygen species for lignocellulose photoreforming. Under full spectrum irradiation for 2 h, the Fe-SA/PCN-HJ exhibits an ultrahigh CO generation rate of 92.33 mmol g-1 and yields 136.21 mg of lactic acid by using 900 mg of fructose as the model substrate. Moreover, we have further demonstrated that the Fe-SA/PCN-HJ photocatalyst presents universally applicable capabilities for the photoreforming of various types of lignocellulosic biomass. This work provides an approach for the production of CO and lactic acid through the photoreforming of lignocellulose, which is promising for the production of fuels and valuable chemicals. Submitted/Accepted version 2025-01-07T05:41:34Z 2025-01-07T05:41:34Z 2024 Journal Article Chen, Y., Zheng, M., Sun, J., Xu, J., Wu, C., Liu, J., He, L., Xi, S., Li, S. & Xue, C. (2024). Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction. ACS Catalysis, 14(23), 17321-17330. https://dx.doi.org/10.1021/acscatal.4c05510 2155-5435 https://hdl.handle.net/10356/182089 10.1021/acscatal.4c05510 2-s2.0-85209544095 23 14 17321 17330 en RG7/23 RG10/21 MOE-T2EP10220-0005 MOE-T2EP20221-0003 ACS Catalysis © 2024 American Chemical Society. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1021/acscatal.4c05510. application/pdf |
| spellingShingle | Chemistry Photoreforming of lignocellulose CO and lactic acid coproduction Chen, Yanglin Zheng, Mei Sun, Jiajun Xu, Jianzhong Wu, Chao Liu, Jiyuan He, Limo Xi, Shibo Li, Shuzhou Xue, Can Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title | Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title_full | Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title_fullStr | Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title_full_unstemmed | Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title_short | Photoreforming of lignocellulose into CO and lactic acid over a single-atom Fe-dispersed order/disorder polymeric carbon nitride homojunction |
| title_sort | photoreforming of lignocellulose into co and lactic acid over a single atom fe dispersed order disorder polymeric carbon nitride homojunction |
| topic | Chemistry Photoreforming of lignocellulose CO and lactic acid coproduction |
| url | https://hdl.handle.net/10356/182089 |
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