Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions
The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH ) ) is conventionally synthesized through two consecutive industrial processes, N + H → NH followed by NH + CO → urea. Both reactions operate under harsh con...
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Veröffentlicht in: | Nature chemistry 2020-08, Vol.12 (8), p.717 |
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creator | Chen, Chen Zhu, Xiaorong Wen, Xiaojian Zhou, Yangyang Zhou, Ling Li, Hao Tao, Li Li, Qiling Du, Shiqian Liu, Tingting Yan, Dafeng Xie, Chao Zou, Yuqin Wang, Yanyong Chen, Ru Huo, Jia Li, Yafei Cheng, Jun Su, Hui Zhao, Xu Cheng, Weiren Liu, Qinghua Lin, Hongzhen Luo, Jun Chen, Jun Dong, Mingdong Cheng, Kai Li, Conggang Wang, Shuangyin |
description | The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH
)
) is conventionally synthesized through two consecutive industrial processes, N
+ H
→ NH
followed by NH
+ CO
→ urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH
produced globally. Here we directly coupled N
and CO
in H
O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO
nanosheets. This coupling reaction occurs through the formation of C-N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g
h
and corresponding Faradic efficiency of 8.92% were measured at -0.4 V versus reversible hydrogen electrode. |
doi_str_mv | 10.1038/s41557-020-0481-9 |
format | Article |
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)
) is conventionally synthesized through two consecutive industrial processes, N
+ H
→ NH
followed by NH
+ CO
→ urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH
produced globally. Here we directly coupled N
and CO
in H
O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO
nanosheets. This coupling reaction occurs through the formation of C-N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g
h
and corresponding Faradic efficiency of 8.92% were measured at -0.4 V versus reversible hydrogen electrode.</description><identifier>EISSN: 1755-4349</identifier><identifier>DOI: 10.1038/s41557-020-0481-9</identifier><identifier>PMID: 32541948</identifier><language>eng</language><publisher>England</publisher><ispartof>Nature chemistry, 2020-08, Vol.12 (8), p.717</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0002-5798-1722 ; 0000-0002-2025-2171 ; 0000-0003-4090-3311 ; 0000-0001-7185-9857 ; 0000-0002-6136-863X ; 0000-0001-5084-2087 ; 0000-0001-6938-6296 ; 0000-0003-2218-7382 ; 0000-0001-6971-0797</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/32541948$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Chen, Chen</creatorcontrib><creatorcontrib>Zhu, Xiaorong</creatorcontrib><creatorcontrib>Wen, Xiaojian</creatorcontrib><creatorcontrib>Zhou, Yangyang</creatorcontrib><creatorcontrib>Zhou, Ling</creatorcontrib><creatorcontrib>Li, Hao</creatorcontrib><creatorcontrib>Tao, Li</creatorcontrib><creatorcontrib>Li, Qiling</creatorcontrib><creatorcontrib>Du, Shiqian</creatorcontrib><creatorcontrib>Liu, Tingting</creatorcontrib><creatorcontrib>Yan, Dafeng</creatorcontrib><creatorcontrib>Xie, Chao</creatorcontrib><creatorcontrib>Zou, Yuqin</creatorcontrib><creatorcontrib>Wang, Yanyong</creatorcontrib><creatorcontrib>Chen, Ru</creatorcontrib><creatorcontrib>Huo, Jia</creatorcontrib><creatorcontrib>Li, Yafei</creatorcontrib><creatorcontrib>Cheng, Jun</creatorcontrib><creatorcontrib>Su, Hui</creatorcontrib><creatorcontrib>Zhao, Xu</creatorcontrib><creatorcontrib>Cheng, Weiren</creatorcontrib><creatorcontrib>Liu, Qinghua</creatorcontrib><creatorcontrib>Lin, Hongzhen</creatorcontrib><creatorcontrib>Luo, Jun</creatorcontrib><creatorcontrib>Chen, Jun</creatorcontrib><creatorcontrib>Dong, Mingdong</creatorcontrib><creatorcontrib>Cheng, Kai</creatorcontrib><creatorcontrib>Li, Conggang</creatorcontrib><creatorcontrib>Wang, Shuangyin</creatorcontrib><title>Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions</title><title>Nature chemistry</title><addtitle>Nat Chem</addtitle><description>The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH
)
) is conventionally synthesized through two consecutive industrial processes, N
+ H
→ NH
followed by NH
+ CO
→ urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH
produced globally. Here we directly coupled N
and CO
in H
O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO
nanosheets. This coupling reaction occurs through the formation of C-N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g
h
and corresponding Faradic efficiency of 8.92% were measured at -0.4 V versus reversible hydrogen electrode.</description><issn>1755-4349</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNqFjb0OgjAYABsTI_jzAC7me4FqS1t-ZqIhDrK4kyJVa6CQFgZ8ehl0drobLjmEtpTsKWHxwXEqRIRJQDDhMcXJDPk0EgJzxhMPLZ17ERIKRsMF8lggOE147KNz2g5drc0DLhCANBWk-STaQDYhh74FN5r-qZx-KxiskjCYSlmQTamV6eHWmkr3ujVujeZ3WTu1-XKFdqfjNc1wN5SNqorO6kbasfjN2d_gAzDBPSI</recordid><startdate>202008</startdate><enddate>202008</enddate><creator>Chen, Chen</creator><creator>Zhu, Xiaorong</creator><creator>Wen, Xiaojian</creator><creator>Zhou, Yangyang</creator><creator>Zhou, Ling</creator><creator>Li, Hao</creator><creator>Tao, Li</creator><creator>Li, Qiling</creator><creator>Du, Shiqian</creator><creator>Liu, Tingting</creator><creator>Yan, Dafeng</creator><creator>Xie, Chao</creator><creator>Zou, Yuqin</creator><creator>Wang, Yanyong</creator><creator>Chen, Ru</creator><creator>Huo, Jia</creator><creator>Li, Yafei</creator><creator>Cheng, Jun</creator><creator>Su, Hui</creator><creator>Zhao, Xu</creator><creator>Cheng, Weiren</creator><creator>Liu, Qinghua</creator><creator>Lin, Hongzhen</creator><creator>Luo, Jun</creator><creator>Chen, Jun</creator><creator>Dong, Mingdong</creator><creator>Cheng, Kai</creator><creator>Li, Conggang</creator><creator>Wang, Shuangyin</creator><scope>NPM</scope><orcidid>https://orcid.org/0000-0002-5798-1722</orcidid><orcidid>https://orcid.org/0000-0002-2025-2171</orcidid><orcidid>https://orcid.org/0000-0003-4090-3311</orcidid><orcidid>https://orcid.org/0000-0001-7185-9857</orcidid><orcidid>https://orcid.org/0000-0002-6136-863X</orcidid><orcidid>https://orcid.org/0000-0001-5084-2087</orcidid><orcidid>https://orcid.org/0000-0001-6938-6296</orcidid><orcidid>https://orcid.org/0000-0003-2218-7382</orcidid><orcidid>https://orcid.org/0000-0001-6971-0797</orcidid></search><sort><creationdate>202008</creationdate><title>Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions</title><author>Chen, Chen ; Zhu, Xiaorong ; Wen, Xiaojian ; Zhou, Yangyang ; Zhou, Ling ; Li, Hao ; Tao, Li ; Li, Qiling ; Du, Shiqian ; Liu, Tingting ; Yan, Dafeng ; Xie, Chao ; Zou, Yuqin ; Wang, Yanyong ; Chen, Ru ; Huo, Jia ; Li, Yafei ; Cheng, Jun ; Su, Hui ; Zhao, Xu ; Cheng, Weiren ; Liu, Qinghua ; Lin, Hongzhen ; Luo, Jun ; Chen, Jun ; Dong, Mingdong ; Cheng, Kai ; Li, Conggang ; Wang, Shuangyin</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-pubmed_primary_325419483</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Chen, Chen</creatorcontrib><creatorcontrib>Zhu, Xiaorong</creatorcontrib><creatorcontrib>Wen, Xiaojian</creatorcontrib><creatorcontrib>Zhou, Yangyang</creatorcontrib><creatorcontrib>Zhou, Ling</creatorcontrib><creatorcontrib>Li, Hao</creatorcontrib><creatorcontrib>Tao, Li</creatorcontrib><creatorcontrib>Li, Qiling</creatorcontrib><creatorcontrib>Du, Shiqian</creatorcontrib><creatorcontrib>Liu, Tingting</creatorcontrib><creatorcontrib>Yan, Dafeng</creatorcontrib><creatorcontrib>Xie, Chao</creatorcontrib><creatorcontrib>Zou, Yuqin</creatorcontrib><creatorcontrib>Wang, Yanyong</creatorcontrib><creatorcontrib>Chen, Ru</creatorcontrib><creatorcontrib>Huo, Jia</creatorcontrib><creatorcontrib>Li, Yafei</creatorcontrib><creatorcontrib>Cheng, Jun</creatorcontrib><creatorcontrib>Su, Hui</creatorcontrib><creatorcontrib>Zhao, Xu</creatorcontrib><creatorcontrib>Cheng, Weiren</creatorcontrib><creatorcontrib>Liu, Qinghua</creatorcontrib><creatorcontrib>Lin, Hongzhen</creatorcontrib><creatorcontrib>Luo, Jun</creatorcontrib><creatorcontrib>Chen, Jun</creatorcontrib><creatorcontrib>Dong, Mingdong</creatorcontrib><creatorcontrib>Cheng, Kai</creatorcontrib><creatorcontrib>Li, Conggang</creatorcontrib><creatorcontrib>Wang, Shuangyin</creatorcontrib><collection>PubMed</collection><jtitle>Nature chemistry</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Chen, Chen</au><au>Zhu, Xiaorong</au><au>Wen, Xiaojian</au><au>Zhou, Yangyang</au><au>Zhou, Ling</au><au>Li, Hao</au><au>Tao, Li</au><au>Li, Qiling</au><au>Du, Shiqian</au><au>Liu, Tingting</au><au>Yan, Dafeng</au><au>Xie, Chao</au><au>Zou, Yuqin</au><au>Wang, Yanyong</au><au>Chen, Ru</au><au>Huo, Jia</au><au>Li, Yafei</au><au>Cheng, Jun</au><au>Su, Hui</au><au>Zhao, Xu</au><au>Cheng, Weiren</au><au>Liu, Qinghua</au><au>Lin, Hongzhen</au><au>Luo, Jun</au><au>Chen, Jun</au><au>Dong, Mingdong</au><au>Cheng, Kai</au><au>Li, Conggang</au><au>Wang, Shuangyin</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions</atitle><jtitle>Nature chemistry</jtitle><addtitle>Nat Chem</addtitle><date>2020-08</date><risdate>2020</risdate><volume>12</volume><issue>8</issue><spage>717</spage><pages>717-</pages><eissn>1755-4349</eissn><abstract>The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH
)
) is conventionally synthesized through two consecutive industrial processes, N
+ H
→ NH
followed by NH
+ CO
→ urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH
produced globally. Here we directly coupled N
and CO
in H
O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO
nanosheets. This coupling reaction occurs through the formation of C-N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g
h
and corresponding Faradic efficiency of 8.92% were measured at -0.4 V versus reversible hydrogen electrode.</abstract><cop>England</cop><pmid>32541948</pmid><doi>10.1038/s41557-020-0481-9</doi><orcidid>https://orcid.org/0000-0002-5798-1722</orcidid><orcidid>https://orcid.org/0000-0002-2025-2171</orcidid><orcidid>https://orcid.org/0000-0003-4090-3311</orcidid><orcidid>https://orcid.org/0000-0001-7185-9857</orcidid><orcidid>https://orcid.org/0000-0002-6136-863X</orcidid><orcidid>https://orcid.org/0000-0001-5084-2087</orcidid><orcidid>https://orcid.org/0000-0001-6938-6296</orcidid><orcidid>https://orcid.org/0000-0003-2218-7382</orcidid><orcidid>https://orcid.org/0000-0001-6971-0797</orcidid></addata></record> |
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title | Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions |
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