{"title":"用于二氧化碳电化学还原的掺钯氧化锡纳米结构催化剂","authors":"Shuting Tan, Zhuo Xiong, Zuwei Xu, Junying Zhang, Yongchun Zhao","doi":"10.1007/s12678-024-00912-8","DOIUrl":null,"url":null,"abstract":"<div><p>Electrocatalytic reduction of CO<sub>2</sub> can convert CO<sub>2</sub> into a variety of carbon-based fuels and achieve carbon neutrality. Tin oxide (SnO<sub>2</sub>) electrocatalytic materials have the advantages of low cost and low toxicity, and the electrocatalytic reduction of CO<sub>2</sub> to formic acid is highly selective. In this paper, Pd-doped SnO<sub>2</sub> nanoparticle materials were synthesized by flame spray pyrolysis and their properties for electrocatalytic reduction of CO<sub>2</sub> to formic acid were explored in a gas diffusion electrolytic cell. The results showed that the Pd/SnO<sub>2</sub> catalysts could improve the catalytic activity for the conversion of CO<sub>2</sub> to formate, and the most superior 0.5 Pd/SnO<sub>2</sub> showed a Faraday efficiency of 63% for formate at − 1.20 V vs. RHE and a current density of 90.59 mA<sup>.</sup>cm<sup>−2</sup>, which were 1.4 and 2.7 times higher than that of pure SnO<sub>2</sub>, respectively. The modified catalyst grains were refined, and the charge transfer resistance at the catalyst interface was reduced, and the electrochemically active area was increased, generating more catalytically active sites and increasing the contact between CO<sub>2</sub>, electrolyte, and electrode-catalyst. Density functional theory calculations showed that the doping of Pd element changed the local structure of SnO<sub>2</sub>, and the Pd/SnO<sub>2</sub> surface was more favorable for the generation of the intermediate products <sup>*</sup>HCOO<sup>−</sup> and formate as well as the inhibition of hydrogen precipitation, which was consistent with the experimental results.</p><h3>Graphical Abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":535,"journal":{"name":"Electrocatalysis","volume":"16 1","pages":"153 - 161"},"PeriodicalIF":2.7000,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Pd-Doped Tin Oxide Nanostructured Catalysts for Electrochemical Reduction of Carbon Dioxide\",\"authors\":\"Shuting Tan, Zhuo Xiong, Zuwei Xu, Junying Zhang, Yongchun Zhao\",\"doi\":\"10.1007/s12678-024-00912-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Electrocatalytic reduction of CO<sub>2</sub> can convert CO<sub>2</sub> into a variety of carbon-based fuels and achieve carbon neutrality. Tin oxide (SnO<sub>2</sub>) electrocatalytic materials have the advantages of low cost and low toxicity, and the electrocatalytic reduction of CO<sub>2</sub> to formic acid is highly selective. In this paper, Pd-doped SnO<sub>2</sub> nanoparticle materials were synthesized by flame spray pyrolysis and their properties for electrocatalytic reduction of CO<sub>2</sub> to formic acid were explored in a gas diffusion electrolytic cell. The results showed that the Pd/SnO<sub>2</sub> catalysts could improve the catalytic activity for the conversion of CO<sub>2</sub> to formate, and the most superior 0.5 Pd/SnO<sub>2</sub> showed a Faraday efficiency of 63% for formate at − 1.20 V vs. RHE and a current density of 90.59 mA<sup>.</sup>cm<sup>−2</sup>, which were 1.4 and 2.7 times higher than that of pure SnO<sub>2</sub>, respectively. The modified catalyst grains were refined, and the charge transfer resistance at the catalyst interface was reduced, and the electrochemically active area was increased, generating more catalytically active sites and increasing the contact between CO<sub>2</sub>, electrolyte, and electrode-catalyst. Density functional theory calculations showed that the doping of Pd element changed the local structure of SnO<sub>2</sub>, and the Pd/SnO<sub>2</sub> surface was more favorable for the generation of the intermediate products <sup>*</sup>HCOO<sup>−</sup> and formate as well as the inhibition of hydrogen precipitation, which was consistent with the experimental results.</p><h3>Graphical Abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":535,\"journal\":{\"name\":\"Electrocatalysis\",\"volume\":\"16 1\",\"pages\":\"153 - 161\"},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-11-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Electrocatalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s12678-024-00912-8\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Electrocatalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s12678-024-00912-8","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
电催化还原二氧化碳可以将二氧化碳转化为多种碳基燃料,实现碳中和。氧化锡(SnO2)电催化材料具有成本低、毒性小等优点,且电催化还原 CO2 为甲酸具有高选择性。本文采用火焰喷射热解法合成了掺杂 Pd 的 SnO2 纳米粒子材料,并在气体扩散电解池中探讨了其电催化还原 CO2 为甲酸的性能。结果表明,Pd/SnO2 催化剂能提高 CO2 转化为甲酸盐的催化活性,其中最优异的 0.5 Pd/SnO2 在 - 1.20 V 对 RHE 条件下,甲酸盐的法拉第效率为 63%,电流密度为 90.59 mA.cm-2,分别是纯 SnO2 的 1.4 倍和 2.7 倍。改性后的催化剂晶粒细化,催化剂界面的电荷转移电阻减小,电化学活性面积增大,产生了更多的催化活性位点,增加了二氧化碳、电解质和电解催化剂之间的接触。密度泛函理论计算表明,掺杂钯元素改变了SnO2的局部结构,Pd/SnO2表面更有利于中间产物*HCOO-和甲酸盐的生成以及抑制氢气的析出,这与实验结果一致。
Pd-Doped Tin Oxide Nanostructured Catalysts for Electrochemical Reduction of Carbon Dioxide
Electrocatalytic reduction of CO2 can convert CO2 into a variety of carbon-based fuels and achieve carbon neutrality. Tin oxide (SnO2) electrocatalytic materials have the advantages of low cost and low toxicity, and the electrocatalytic reduction of CO2 to formic acid is highly selective. In this paper, Pd-doped SnO2 nanoparticle materials were synthesized by flame spray pyrolysis and their properties for electrocatalytic reduction of CO2 to formic acid were explored in a gas diffusion electrolytic cell. The results showed that the Pd/SnO2 catalysts could improve the catalytic activity for the conversion of CO2 to formate, and the most superior 0.5 Pd/SnO2 showed a Faraday efficiency of 63% for formate at − 1.20 V vs. RHE and a current density of 90.59 mA.cm−2, which were 1.4 and 2.7 times higher than that of pure SnO2, respectively. The modified catalyst grains were refined, and the charge transfer resistance at the catalyst interface was reduced, and the electrochemically active area was increased, generating more catalytically active sites and increasing the contact between CO2, electrolyte, and electrode-catalyst. Density functional theory calculations showed that the doping of Pd element changed the local structure of SnO2, and the Pd/SnO2 surface was more favorable for the generation of the intermediate products *HCOO− and formate as well as the inhibition of hydrogen precipitation, which was consistent with the experimental results.
期刊介绍:
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