Loading…
Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia
The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis to provide an efficient and clean process for recovera...
Saved in:
Published in: | Advanced energy materials 2023-05, Vol.13 (20), p.n/a |
---|---|
Main Authors: | , , , , , , |
Format: | Article |
Language: | English |
Subjects: | |
Citations: | Items that this one cites Items that cite this one |
Online Access: | Get full text |
Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
cited_by | cdi_FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3 |
---|---|
cites | cdi_FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3 |
container_end_page | n/a |
container_issue | 20 |
container_start_page | |
container_title | Advanced energy materials |
container_volume | 13 |
creator | Zhu, Xuefang Fan, Xing Lin, Haiping Li, Shuni Zhai, Quanguo Jiang, Yucheng Chen, Yu |
description | The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis to provide an efficient and clean process for recoverable ammonia production. NO2− is reduced to NH3 by electroenzymatic cascade reduction reaction on a bioconjugate, in which 1‐butyl‐3‐methylimidazolium bromide (ILBMB) modified chloroperoxidase (CPO) is fixed on polyethyleneimine (PEI) modified multi‐walled carbon nanotubes (MWCNT) to from bioconjugate (CPO‐ILBMB/MWCNT‐PEI). 15N and 14N isotope labeling reveal that the NH3 species is derived from NO2− reduction. Density functional theory calculations identify that the FeII species in heme center of CPO serve as the key active site for NO2− reduction. The amino groups derived from MWCNT‐PEI not only serve as a bridge to covalently immobilize CPO but also enrich the NO2− ion at electrode/solution interface through electrostatic interactions. The low energy barrier of NO2− reduction and low adsorption free energy of the intermediate result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in pH 5.0 solution. The highly efficient electroenzymatic reaction ensurespromising applications in the conversion of NO2− to NH3.
Electrocatalysis combine with enzymatic catalysis to provide an efficient and clean process for nitrite reduction. The NO2– is effectively reduced to ammonia at a CPO‐ILBMB/MWCNT‐PEI bioconjugate by electroenzymatic cascade catalysis. The low energy barrier and low adsorption‐free energy result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in near‐neutral solution. |
doi_str_mv | 10.1002/aenm.202300669 |
format | article |
fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2818599811</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2818599811</sourcerecordid><originalsourceid>FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3</originalsourceid><addsrcrecordid>eNqFkM1Lw0AQxYMoWGqvnhc8p-5HsskeS0mtUCtIPS_bzcRuSbJ1d6vEv96EiB6dy_wY3psZXhTdEjwnGNN7BW0zp5gyjDkXF9GEcJLEPE_w5S8zeh3NvD_ivhJBMGOTCNbm7VB3qKgqow20ARU16OAstF9do4LRaKm8ViWgFyjPOhjb9qRGWFmHdgdAS9t-gPPDyFZoa4IzAVCwaNE0tjXqJrqqVO1h9tOn0euq2C3X8eb54XG52MSakUzEw5_JXmnOkowqXGU6JyxNRIIpT7HIWMq5woKUUGlFNSn3XJUUSkJxnuI9sGl0N-49Oft-Bh_k0Z5d25-UNCd5KkROSK-ajyrtrPcOKnlyplGukwTLIU05pCl_0-wNYjR8mhq6f9RyUWyf_rzf_SJ4WQ</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2818599811</pqid></control><display><type>article</type><title>Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia</title><source>Wiley</source><creator>Zhu, Xuefang ; Fan, Xing ; Lin, Haiping ; Li, Shuni ; Zhai, Quanguo ; Jiang, Yucheng ; Chen, Yu</creator><creatorcontrib>Zhu, Xuefang ; Fan, Xing ; Lin, Haiping ; Li, Shuni ; Zhai, Quanguo ; Jiang, Yucheng ; Chen, Yu</creatorcontrib><description>The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis to provide an efficient and clean process for recoverable ammonia production. NO2− is reduced to NH3 by electroenzymatic cascade reduction reaction on a bioconjugate, in which 1‐butyl‐3‐methylimidazolium bromide (ILBMB) modified chloroperoxidase (CPO) is fixed on polyethyleneimine (PEI) modified multi‐walled carbon nanotubes (MWCNT) to from bioconjugate (CPO‐ILBMB/MWCNT‐PEI). 15N and 14N isotope labeling reveal that the NH3 species is derived from NO2− reduction. Density functional theory calculations identify that the FeII species in heme center of CPO serve as the key active site for NO2− reduction. The amino groups derived from MWCNT‐PEI not only serve as a bridge to covalently immobilize CPO but also enrich the NO2− ion at electrode/solution interface through electrostatic interactions. The low energy barrier of NO2− reduction and low adsorption free energy of the intermediate result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in pH 5.0 solution. The highly efficient electroenzymatic reaction ensurespromising applications in the conversion of NO2− to NH3.
Electrocatalysis combine with enzymatic catalysis to provide an efficient and clean process for nitrite reduction. The NO2– is effectively reduced to ammonia at a CPO‐ILBMB/MWCNT‐PEI bioconjugate by electroenzymatic cascade catalysis. The low energy barrier and low adsorption‐free energy result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in near‐neutral solution.</description><identifier>ISSN: 1614-6832</identifier><identifier>EISSN: 1614-6840</identifier><identifier>DOI: 10.1002/aenm.202300669</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Ammonia ; ammonia synthesis ; Chemical reduction ; chloroperoxidase ; Conversion ; Density functional theory ; electroenzymatic cascade reduction reaction ; Free energy ; Multi wall carbon nanotubes ; nitrate reduction reaction ; Nitrogen dioxide ; Nitrogen isotopes ; Polyethyleneimine ; selectivity</subject><ispartof>Advanced energy materials, 2023-05, Vol.13 (20), p.n/a</ispartof><rights>2023 Wiley‐VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3</citedby><cites>FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3</cites><orcidid>0000-0002-9936-3893 ; 0000-0001-9545-6761</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Faenm.202300669$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Faenm.202300669$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>315,786,790,27957,27958,50923,51032</link.rule.ids></links><search><creatorcontrib>Zhu, Xuefang</creatorcontrib><creatorcontrib>Fan, Xing</creatorcontrib><creatorcontrib>Lin, Haiping</creatorcontrib><creatorcontrib>Li, Shuni</creatorcontrib><creatorcontrib>Zhai, Quanguo</creatorcontrib><creatorcontrib>Jiang, Yucheng</creatorcontrib><creatorcontrib>Chen, Yu</creatorcontrib><title>Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia</title><title>Advanced energy materials</title><description>The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis to provide an efficient and clean process for recoverable ammonia production. NO2− is reduced to NH3 by electroenzymatic cascade reduction reaction on a bioconjugate, in which 1‐butyl‐3‐methylimidazolium bromide (ILBMB) modified chloroperoxidase (CPO) is fixed on polyethyleneimine (PEI) modified multi‐walled carbon nanotubes (MWCNT) to from bioconjugate (CPO‐ILBMB/MWCNT‐PEI). 15N and 14N isotope labeling reveal that the NH3 species is derived from NO2− reduction. Density functional theory calculations identify that the FeII species in heme center of CPO serve as the key active site for NO2− reduction. The amino groups derived from MWCNT‐PEI not only serve as a bridge to covalently immobilize CPO but also enrich the NO2− ion at electrode/solution interface through electrostatic interactions. The low energy barrier of NO2− reduction and low adsorption free energy of the intermediate result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in pH 5.0 solution. The highly efficient electroenzymatic reaction ensurespromising applications in the conversion of NO2− to NH3.
Electrocatalysis combine with enzymatic catalysis to provide an efficient and clean process for nitrite reduction. The NO2– is effectively reduced to ammonia at a CPO‐ILBMB/MWCNT‐PEI bioconjugate by electroenzymatic cascade catalysis. The low energy barrier and low adsorption‐free energy result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in near‐neutral solution.</description><subject>Ammonia</subject><subject>ammonia synthesis</subject><subject>Chemical reduction</subject><subject>chloroperoxidase</subject><subject>Conversion</subject><subject>Density functional theory</subject><subject>electroenzymatic cascade reduction reaction</subject><subject>Free energy</subject><subject>Multi wall carbon nanotubes</subject><subject>nitrate reduction reaction</subject><subject>Nitrogen dioxide</subject><subject>Nitrogen isotopes</subject><subject>Polyethyleneimine</subject><subject>selectivity</subject><issn>1614-6832</issn><issn>1614-6840</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkM1Lw0AQxYMoWGqvnhc8p-5HsskeS0mtUCtIPS_bzcRuSbJ1d6vEv96EiB6dy_wY3psZXhTdEjwnGNN7BW0zp5gyjDkXF9GEcJLEPE_w5S8zeh3NvD_ivhJBMGOTCNbm7VB3qKgqow20ARU16OAstF9do4LRaKm8ViWgFyjPOhjb9qRGWFmHdgdAS9t-gPPDyFZoa4IzAVCwaNE0tjXqJrqqVO1h9tOn0euq2C3X8eb54XG52MSakUzEw5_JXmnOkowqXGU6JyxNRIIpT7HIWMq5woKUUGlFNSn3XJUUSkJxnuI9sGl0N-49Oft-Bh_k0Z5d25-UNCd5KkROSK-ajyrtrPcOKnlyplGukwTLIU05pCl_0-wNYjR8mhq6f9RyUWyf_rzf_SJ4WQ</recordid><startdate>20230501</startdate><enddate>20230501</enddate><creator>Zhu, Xuefang</creator><creator>Fan, Xing</creator><creator>Lin, Haiping</creator><creator>Li, Shuni</creator><creator>Zhai, Quanguo</creator><creator>Jiang, Yucheng</creator><creator>Chen, Yu</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SP</scope><scope>7TB</scope><scope>8FD</scope><scope>F28</scope><scope>FR3</scope><scope>H8D</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0002-9936-3893</orcidid><orcidid>https://orcid.org/0000-0001-9545-6761</orcidid></search><sort><creationdate>20230501</creationdate><title>Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia</title><author>Zhu, Xuefang ; Fan, Xing ; Lin, Haiping ; Li, Shuni ; Zhai, Quanguo ; Jiang, Yucheng ; Chen, Yu</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Ammonia</topic><topic>ammonia synthesis</topic><topic>Chemical reduction</topic><topic>chloroperoxidase</topic><topic>Conversion</topic><topic>Density functional theory</topic><topic>electroenzymatic cascade reduction reaction</topic><topic>Free energy</topic><topic>Multi wall carbon nanotubes</topic><topic>nitrate reduction reaction</topic><topic>Nitrogen dioxide</topic><topic>Nitrogen isotopes</topic><topic>Polyethyleneimine</topic><topic>selectivity</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhu, Xuefang</creatorcontrib><creatorcontrib>Fan, Xing</creatorcontrib><creatorcontrib>Lin, Haiping</creatorcontrib><creatorcontrib>Li, Shuni</creatorcontrib><creatorcontrib>Zhai, Quanguo</creatorcontrib><creatorcontrib>Jiang, Yucheng</creatorcontrib><creatorcontrib>Chen, Yu</creatorcontrib><collection>CrossRef</collection><collection>Electronics & Communications Abstracts</collection><collection>Mechanical & Transportation Engineering Abstracts</collection><collection>Technology Research Database</collection><collection>ANTE: Abstracts in New Technology & Engineering</collection><collection>Engineering Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Advanced energy materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhu, Xuefang</au><au>Fan, Xing</au><au>Lin, Haiping</au><au>Li, Shuni</au><au>Zhai, Quanguo</au><au>Jiang, Yucheng</au><au>Chen, Yu</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia</atitle><jtitle>Advanced energy materials</jtitle><date>2023-05-01</date><risdate>2023</risdate><volume>13</volume><issue>20</issue><epage>n/a</epage><issn>1614-6832</issn><eissn>1614-6840</eissn><abstract>The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis to provide an efficient and clean process for recoverable ammonia production. NO2− is reduced to NH3 by electroenzymatic cascade reduction reaction on a bioconjugate, in which 1‐butyl‐3‐methylimidazolium bromide (ILBMB) modified chloroperoxidase (CPO) is fixed on polyethyleneimine (PEI) modified multi‐walled carbon nanotubes (MWCNT) to from bioconjugate (CPO‐ILBMB/MWCNT‐PEI). 15N and 14N isotope labeling reveal that the NH3 species is derived from NO2− reduction. Density functional theory calculations identify that the FeII species in heme center of CPO serve as the key active site for NO2− reduction. The amino groups derived from MWCNT‐PEI not only serve as a bridge to covalently immobilize CPO but also enrich the NO2− ion at electrode/solution interface through electrostatic interactions. The low energy barrier of NO2− reduction and low adsorption free energy of the intermediate result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in pH 5.0 solution. The highly efficient electroenzymatic reaction ensurespromising applications in the conversion of NO2− to NH3.
Electrocatalysis combine with enzymatic catalysis to provide an efficient and clean process for nitrite reduction. The NO2– is effectively reduced to ammonia at a CPO‐ILBMB/MWCNT‐PEI bioconjugate by electroenzymatic cascade catalysis. The low energy barrier and low adsorption‐free energy result in high Faradaic efficiency (96.4%), NH3 yield (112.7 mg h−1 mgCPO−1), and high selectivity in near‐neutral solution.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/aenm.202300669</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0002-9936-3893</orcidid><orcidid>https://orcid.org/0000-0001-9545-6761</orcidid></addata></record> |
fulltext | fulltext |
identifier | ISSN: 1614-6832 |
ispartof | Advanced energy materials, 2023-05, Vol.13 (20), p.n/a |
issn | 1614-6832 1614-6840 |
language | eng |
recordid | cdi_proquest_journals_2818599811 |
source | Wiley |
subjects | Ammonia ammonia synthesis Chemical reduction chloroperoxidase Conversion Density functional theory electroenzymatic cascade reduction reaction Free energy Multi wall carbon nanotubes nitrate reduction reaction Nitrogen dioxide Nitrogen isotopes Polyethyleneimine selectivity |
title | Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia |
url | http://sfxeu10.hosted.exlibrisgroup.com/loughborough?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-09-21T20%3A22%3A20IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Highly%20Efficient%20Electroenzymatic%20Cascade%20Reduction%20Reaction%20For%20The%20Conversion%20of%20Nitrite%20to%20Ammonia&rft.jtitle=Advanced%20energy%20materials&rft.au=Zhu,%20Xuefang&rft.date=2023-05-01&rft.volume=13&rft.issue=20&rft.epage=n/a&rft.issn=1614-6832&rft.eissn=1614-6840&rft_id=info:doi/10.1002/aenm.202300669&rft_dat=%3Cproquest_cross%3E2818599811%3C/proquest_cross%3E%3Cgrp_id%3Ecdi_FETCH-LOGICAL-c3179-16144bac63472a0f7c813549402650973566a091defca2c1db6ad2ed120850be3%3C/grp_id%3E%3Coa%3E%3C/oa%3E%3Curl%3E%3C/url%3E&rft_id=info:oai/&rft_pqid=2818599811&rft_id=info:pmid/&rfr_iscdi=true |