Additive-free CO2 hydrogenation to pure formic acid solution via amine-modified Pd catalyst at room temperature
Direct conversion of CO2 into pure formic acid (FA) solution in the absence of base additives is of great significance, but is challenging due to thermodynamic limitations. Here, we have synthesized ultrafine Pd nano-catalysts modified with three kinds of amine groups, including a primary amine (PA)...
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| Veröffentlicht in: | Green chemistry : an international journal and green chemistry resource : GC 2023-07, Vol.25 (15), p.6025-6031 |
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| container_title | Green chemistry : an international journal and green chemistry resource : GC |
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| creator | Jiang, Shuchao Liu, Xiaokong Zhai, Shengliang Ci, Xiuqin Yu, Tie Sun, Lei Zhai, Dong Deng, Weiqiao Ren, Guoqing |
| description | Direct conversion of CO2 into pure formic acid (FA) solution in the absence of base additives is of great significance, but is challenging due to thermodynamic limitations. Here, we have synthesized ultrafine Pd nano-catalysts modified with three kinds of amine groups, including a primary amine (PA), secondary amine (SA) and tertiary amine (TA), which realized the efficient hydrogenation of CO2 to pure FA in water at room temperature for the first time. Comprehensive characterizations reveal that all the amine groups are beneficial to the formation of ultrafine and uniform Pd nanoclusters ( |
| doi_str_mv | 10.1039/d3gc01307c |
| format | Article |
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Here, we have synthesized ultrafine Pd nano-catalysts modified with three kinds of amine groups, including a primary amine (PA), secondary amine (SA) and tertiary amine (TA), which realized the efficient hydrogenation of CO2 to pure FA in water at room temperature for the first time. Comprehensive characterizations reveal that all the amine groups are beneficial to the formation of ultrafine and uniform Pd nanoclusters (<2 nm), and that the electron-richness of Pd has a competitive effect with the steric hindrance of the amine groups on the CO2 hydrogenation activity. The SA-modified catalyst Pd/AC-SA, which has a lower binding energy of N and lower steric hindrance, thus shows the best turnover frequency (TOF) of 29.1 h−1 at 298 K and 4.0 MPa, which is even comparable to that of reported heterogeneous catalysts with base additives under harsh conditions. The DFT calculations further revealed the mechanism of CO2 hydrogenation; the first H-atom hydrogenation is the rate-determining step, which is in good agreement with the experiments. This work, as a successful example of the direct generation of pure FA solution at room temperature, exhibits great potential for future large-scale hydrogen storage.</description><identifier>ISSN: 1463-9262</identifier><identifier>EISSN: 1463-9270</identifier><identifier>DOI: 10.1039/d3gc01307c</identifier><language>eng</language><publisher>Cambridge: Royal Society of Chemistry</publisher><subject>Additives ; Carbon dioxide ; Catalysts ; Chemical synthesis ; Direct conversion ; Formic acid ; Green chemistry ; Hydrogen storage ; Hydrogenation ; Nanoclusters ; Room temperature ; Steric hindrance ; Ultrafines</subject><ispartof>Green chemistry : an international journal and green chemistry resource : GC, 2023-07, Vol.25 (15), p.6025-6031</ispartof><rights>Copyright Royal Society of Chemistry 2023</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27903,27904</link.rule.ids></links><search><creatorcontrib>Jiang, Shuchao</creatorcontrib><creatorcontrib>Liu, Xiaokong</creatorcontrib><creatorcontrib>Zhai, Shengliang</creatorcontrib><creatorcontrib>Ci, Xiuqin</creatorcontrib><creatorcontrib>Yu, Tie</creatorcontrib><creatorcontrib>Sun, Lei</creatorcontrib><creatorcontrib>Zhai, Dong</creatorcontrib><creatorcontrib>Deng, Weiqiao</creatorcontrib><creatorcontrib>Ren, Guoqing</creatorcontrib><title>Additive-free CO2 hydrogenation to pure formic acid solution via amine-modified Pd catalyst at room temperature</title><title>Green chemistry : an international journal and green chemistry resource : GC</title><description>Direct conversion of CO2 into pure formic acid (FA) solution in the absence of base additives is of great significance, but is challenging due to thermodynamic limitations. Here, we have synthesized ultrafine Pd nano-catalysts modified with three kinds of amine groups, including a primary amine (PA), secondary amine (SA) and tertiary amine (TA), which realized the efficient hydrogenation of CO2 to pure FA in water at room temperature for the first time. Comprehensive characterizations reveal that all the amine groups are beneficial to the formation of ultrafine and uniform Pd nanoclusters (<2 nm), and that the electron-richness of Pd has a competitive effect with the steric hindrance of the amine groups on the CO2 hydrogenation activity. The SA-modified catalyst Pd/AC-SA, which has a lower binding energy of N and lower steric hindrance, thus shows the best turnover frequency (TOF) of 29.1 h−1 at 298 K and 4.0 MPa, which is even comparable to that of reported heterogeneous catalysts with base additives under harsh conditions. The DFT calculations further revealed the mechanism of CO2 hydrogenation; the first H-atom hydrogenation is the rate-determining step, which is in good agreement with the experiments. This work, as a successful example of the direct generation of pure FA solution at room temperature, exhibits great potential for future large-scale hydrogen storage.</description><subject>Additives</subject><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>Chemical synthesis</subject><subject>Direct conversion</subject><subject>Formic acid</subject><subject>Green chemistry</subject><subject>Hydrogen storage</subject><subject>Hydrogenation</subject><subject>Nanoclusters</subject><subject>Room temperature</subject><subject>Steric hindrance</subject><subject>Ultrafines</subject><issn>1463-9262</issn><issn>1463-9270</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNo9kE1LAzEURYMoWKsbf0HA9Wi-JpksS1ErFOpC1-WZvNSUzmTMZAr99w4qru6BC-fCJeSWs3vOpH3wcucYl8y4MzLjSsvKCsPO_1mLS3I1DHvGODdazUhaeB9LPGIVMiJdbgT9PPmcdthBiamjJdF-zEhDym10FFz0dEiH8ac8RqDQxg6rNvkYInr66qmDAofTUCgUmlNqacG2xwxl8lyTiwCHAW_-ck7enx7flqtqvXl-WS7WVc8bWSoIKIyqa-GkRq-0qSEoayxDboJTSngt6sZ462rptfwA3TiNXIGsrWTo5Zzc_Xr7nL5GHMp2n8bcTZNb0SjZKGanw74BzOlbpA</recordid><startdate>20230731</startdate><enddate>20230731</enddate><creator>Jiang, Shuchao</creator><creator>Liu, Xiaokong</creator><creator>Zhai, Shengliang</creator><creator>Ci, Xiuqin</creator><creator>Yu, Tie</creator><creator>Sun, Lei</creator><creator>Zhai, Dong</creator><creator>Deng, Weiqiao</creator><creator>Ren, Guoqing</creator><general>Royal Society of Chemistry</general><scope>7SR</scope><scope>7ST</scope><scope>7U6</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>JG9</scope></search><sort><creationdate>20230731</creationdate><title>Additive-free CO2 hydrogenation to pure formic acid solution via amine-modified Pd catalyst at room temperature</title><author>Jiang, Shuchao ; Liu, Xiaokong ; Zhai, Shengliang ; Ci, Xiuqin ; Yu, Tie ; Sun, Lei ; Zhai, Dong ; Deng, Weiqiao ; Ren, Guoqing</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-p183t-afe274552c36ed4675af49790e17fc442d62587d9c53d63ba68c6e14a35930ed3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Additives</topic><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>Chemical synthesis</topic><topic>Direct conversion</topic><topic>Formic acid</topic><topic>Green chemistry</topic><topic>Hydrogen storage</topic><topic>Hydrogenation</topic><topic>Nanoclusters</topic><topic>Room temperature</topic><topic>Steric hindrance</topic><topic>Ultrafines</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Jiang, Shuchao</creatorcontrib><creatorcontrib>Liu, Xiaokong</creatorcontrib><creatorcontrib>Zhai, Shengliang</creatorcontrib><creatorcontrib>Ci, Xiuqin</creatorcontrib><creatorcontrib>Yu, Tie</creatorcontrib><creatorcontrib>Sun, Lei</creatorcontrib><creatorcontrib>Zhai, Dong</creatorcontrib><creatorcontrib>Deng, Weiqiao</creatorcontrib><creatorcontrib>Ren, Guoqing</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>Environment Abstracts</collection><collection>Sustainability Science Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Environmental Sciences and Pollution Management</collection><collection>Materials Research Database</collection><jtitle>Green chemistry : an international journal and green chemistry resource : GC</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Jiang, Shuchao</au><au>Liu, Xiaokong</au><au>Zhai, Shengliang</au><au>Ci, Xiuqin</au><au>Yu, Tie</au><au>Sun, Lei</au><au>Zhai, Dong</au><au>Deng, Weiqiao</au><au>Ren, Guoqing</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Additive-free CO2 hydrogenation to pure formic acid solution via amine-modified Pd catalyst at room temperature</atitle><jtitle>Green chemistry : an international journal and green chemistry resource : GC</jtitle><date>2023-07-31</date><risdate>2023</risdate><volume>25</volume><issue>15</issue><spage>6025</spage><epage>6031</epage><pages>6025-6031</pages><issn>1463-9262</issn><eissn>1463-9270</eissn><abstract>Direct conversion of CO2 into pure formic acid (FA) solution in the absence of base additives is of great significance, but is challenging due to thermodynamic limitations. Here, we have synthesized ultrafine Pd nano-catalysts modified with three kinds of amine groups, including a primary amine (PA), secondary amine (SA) and tertiary amine (TA), which realized the efficient hydrogenation of CO2 to pure FA in water at room temperature for the first time. Comprehensive characterizations reveal that all the amine groups are beneficial to the formation of ultrafine and uniform Pd nanoclusters (<2 nm), and that the electron-richness of Pd has a competitive effect with the steric hindrance of the amine groups on the CO2 hydrogenation activity. The SA-modified catalyst Pd/AC-SA, which has a lower binding energy of N and lower steric hindrance, thus shows the best turnover frequency (TOF) of 29.1 h−1 at 298 K and 4.0 MPa, which is even comparable to that of reported heterogeneous catalysts with base additives under harsh conditions. The DFT calculations further revealed the mechanism of CO2 hydrogenation; the first H-atom hydrogenation is the rate-determining step, which is in good agreement with the experiments. This work, as a successful example of the direct generation of pure FA solution at room temperature, exhibits great potential for future large-scale hydrogen storage.</abstract><cop>Cambridge</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d3gc01307c</doi><tpages>7</tpages></addata></record> |
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| source | Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
| subjects | Additives Carbon dioxide Catalysts Chemical synthesis Direct conversion Formic acid Green chemistry Hydrogen storage Hydrogenation Nanoclusters Room temperature Steric hindrance Ultrafines |
| title | Additive-free CO2 hydrogenation to pure formic acid solution via amine-modified Pd catalyst at room temperature |
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