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Synergy of Pd2+/S2−-Doped TiO2 Supported on 2-Methylimidazolium-Functionalized Polypyrrole/Graphene Oxide for Enhanced Nitrogen Electrooxidation
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-16 , DOI: 10.1002/adma.202313155
Hui Mao 1, 2 , Yuheng Sun 1 , Huinan Li 1 , Shuyao Wu 1 , Daliang Liu 1 , Hui Li 2 , Shuo Li 1 , Tianyi Ma 2
Advanced Materials ( IF 27.4 ) Pub Date : 2024-01-16 , DOI: 10.1002/adma.202313155
Hui Mao 1, 2 , Yuheng Sun 1 , Huinan Li 1 , Shuyao Wu 1 , Daliang Liu 1 , Hui Li 2 , Shuo Li 1 , Tianyi Ma 2
Affiliation
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The electrosynthesis of nitrate catalyzed by electrochemical nitrogen oxidation reaction (NOR) is considered as an alternative and sustainable approach to the conventional industrial manufacture, but optimizing the electrocatalytic NOR performance and fabricating the efficient NOR electrocatalysts at the design level still encounter great challenges. Herein, unique Pd2+- and S2−-doped TiO2 (Pb/S–TiO2) nanoparticles are successfully in situ grown on the surface of 2-methylimidazolium-functionalized polypyrrole/graphene oxide (2-MeIm/PPy/GO), which present the typical hierarchical micro-nanostructures, resulting in the excellent electrocatalytic NOR performance with the highest NO3− yield of 72.69 µg h−1 mg−1act. and the maximum Faraday efficiency of 8.92% at 2.04 V (vs reversible hydrogen electrode) due to the synergistic effect of each component. Due to the doping effect, the appropriate oxygen evolution reaction (OER) activity is achieved by Ti-site, where OER principally occurs, providing *O during the non-electrochemical step of NOR, while the electrocatalytic NOR process as the electrochemical conversion of inert N2 to active *NO intermediates mainly occurs at the Pd-site. Especially, the sulfate radicals in situ formed on Pb/S–TiO2@2-MeIm/PPy/GO further promote nitrogen adsorption and decrease the reaction energy barrier, resulting in the acceleration of NOR. It provides theoretical and practical experience for the design and preparation of NOR electrocatalysts.
中文翻译：
2-甲基咪唑鎓功能化聚吡咯/氧化石墨烯负载 Pd2+/S2−掺杂 TiO2 的协同作用增强氮电氧化
电化学氮氧化反应（NOR）催化电合成硝酸盐被认为是传统工业制造的一种替代且可持续的方法，但在设计层面优化电催化NOR性能并制造高效的NOR电催化剂仍面临巨大挑战。在此，独特的Pd 2+和S 2−掺杂的TiO 2 (Pb/S–TiO 2 )纳米颗粒成功地在2-甲基咪唑功能化的聚吡咯/氧化石墨烯(2-MeIm/PPy/GO)的表面上原位生长。 ），呈现出典型的分级微纳米结构，从而产生优异的电催化NOR性能，最高NO 3 -产量为72.69 µg h -1 mg -1 act。由于每个组件的协同效应，在 2.04 V（相对于可逆氢电极）时最大法拉第效率为 8.92%。由于掺杂效应，Ti位点实现了适当的析氧反应（OER）活性，其中主要发生OER，在NOR的非电化学步骤中提供*O，而电催化NOR过程作为惰性物质的电化学转化N 2到活性*NO中间体主要发生在Pd位点。特别是，Pb/S–TiO 2 @2-MeIm/PPy/GO上原位形成的硫酸根进一步促进氮吸附并降低反应能垒，从而加速NOR。为NOR电催化剂的设计和制备提供理论和实践经验。
更新日期：2024-01-16
中文翻译：
2-甲基咪唑鎓功能化聚吡咯/氧化石墨烯负载 Pd2+/S2−掺杂 TiO2 的协同作用增强氮电氧化
电化学氮氧化反应（NOR）催化电合成硝酸盐被认为是传统工业制造的一种替代且可持续的方法，但在设计层面优化电催化NOR性能并制造高效的NOR电催化剂仍面临巨大挑战。在此，独特的Pd 2+和S 2−掺杂的TiO 2 (Pb/S–TiO 2 )纳米颗粒成功地在2-甲基咪唑功能化的聚吡咯/氧化石墨烯(2-MeIm/PPy/GO)的表面上原位生长。 ），呈现出典型的分级微纳米结构，从而产生优异的电催化NOR性能，最高NO 3 -产量为72.69 µg h -1 mg -1 act。由于每个组件的协同效应，在 2.04 V（相对于可逆氢电极）时最大法拉第效率为 8.92%。由于掺杂效应，Ti位点实现了适当的析氧反应（OER）活性，其中主要发生OER，在NOR的非电化学步骤中提供*O，而电催化NOR过程作为惰性物质的电化学转化N 2到活性*NO中间体主要发生在Pd位点。特别是，Pb/S–TiO 2 @2-MeIm/PPy/GO上原位形成的硫酸根进一步促进氮吸附并降低反应能垒，从而加速NOR。为NOR电催化剂的设计和制备提供理论和实践经验。
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