Jefferson Honorio Franco, João Victor Bonaldo, Shelley D Minteer, Adalgisa R De Andrade
{"title":"基于混合酶/双金属复合材料的全乳酸催化电氧化增强生物燃料电池。","authors":"Jefferson Honorio Franco, João Victor Bonaldo, Shelley D Minteer, Adalgisa R De Andrade","doi":"10.1021/acsmaterialsau.5c00039","DOIUrl":null,"url":null,"abstract":"<p><p>We describe complete lactate electrooxidation in an enzymatic biofuel cell that combines the catalytic action of the bimetallic composite Ru@Pt-CNT and the enzyme oxalate oxidase (OxOx). The Ru@Pt-CNT/OxOx hybrid electrode was 2.0-fold more catalytically active than the electrode containing the bimetallic composite only. During chronoamperometric experiments, the hybrid electrode achieved a 35% higher maximum current density (2.65 ± 0.15 mA cm<sup>-2</sup>) than the Ru@Pt-CNT electrode. Electrochemical impedance spectroscopy showed that the hybrid electrode had lower charge transfer resistance than the Ru@Pt-CNT electrode, confirming that OxOx had a high affinity for lactate during the bioelectrocatalytic reaction on the electrode surface. Furthermore, 18-h long-term bulk electrolysis revealed that lactate electrooxidation at the Ru@Pt-CNT/OxOx hybrid electrode provided a total charge of 1.2 ± 0.2 C, which was 3-fold higher than the total charge generated by the Ru@Pt-CNT electrode. The lactate oxidation products generated at the hybrid electrode were detected during bulk electrolysis by chromatography, which showed that the hybrid biofilm harvested all 10 electrons from lactate, completely oxidizing it to CO<sub>2</sub>. With exceptional stability and catalytic performance, the hybrid electrode acted in the multiple catabolic steps of lactate oxidation. Overall, the interaction between Ru@Pt-CNT and OxOx enhanced the assembly of lactate biofuel cells to improve lactate electrooxidation. This could pave the way for developing efficient electronic devices with promising applications in bioelectrochemistry.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 4","pages":"732-742"},"PeriodicalIF":6.5000,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12257398/pdf/","citationCount":"0","resultStr":"{\"title\":\"Enhanced Biofuel Cells Based on a Hybrid Enzymatic/Bimetallic Composite for Complete Lactate Catalytic Electrooxidation.\",\"authors\":\"Jefferson Honorio Franco, João Victor Bonaldo, Shelley D Minteer, Adalgisa R De Andrade\",\"doi\":\"10.1021/acsmaterialsau.5c00039\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>We describe complete lactate electrooxidation in an enzymatic biofuel cell that combines the catalytic action of the bimetallic composite Ru@Pt-CNT and the enzyme oxalate oxidase (OxOx). The Ru@Pt-CNT/OxOx hybrid electrode was 2.0-fold more catalytically active than the electrode containing the bimetallic composite only. During chronoamperometric experiments, the hybrid electrode achieved a 35% higher maximum current density (2.65 ± 0.15 mA cm<sup>-2</sup>) than the Ru@Pt-CNT electrode. Electrochemical impedance spectroscopy showed that the hybrid electrode had lower charge transfer resistance than the Ru@Pt-CNT electrode, confirming that OxOx had a high affinity for lactate during the bioelectrocatalytic reaction on the electrode surface. Furthermore, 18-h long-term bulk electrolysis revealed that lactate electrooxidation at the Ru@Pt-CNT/OxOx hybrid electrode provided a total charge of 1.2 ± 0.2 C, which was 3-fold higher than the total charge generated by the Ru@Pt-CNT electrode. The lactate oxidation products generated at the hybrid electrode were detected during bulk electrolysis by chromatography, which showed that the hybrid biofilm harvested all 10 electrons from lactate, completely oxidizing it to CO<sub>2</sub>. With exceptional stability and catalytic performance, the hybrid electrode acted in the multiple catabolic steps of lactate oxidation. Overall, the interaction between Ru@Pt-CNT and OxOx enhanced the assembly of lactate biofuel cells to improve lactate electrooxidation. This could pave the way for developing efficient electronic devices with promising applications in bioelectrochemistry.</p>\",\"PeriodicalId\":29798,\"journal\":{\"name\":\"ACS Materials Au\",\"volume\":\"5 4\",\"pages\":\"732-742\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2025-06-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12257398/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Materials Au\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1021/acsmaterialsau.5c00039\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/7/9 0:00:00\",\"PubModel\":\"eCollection\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Materials Au","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1021/acsmaterialsau.5c00039","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/7/9 0:00:00","PubModel":"eCollection","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
我们描述了在酶生物燃料电池中完全乳酸电氧化,该电池结合了双金属复合材料Ru@Pt-CNT和草酸氧化酶(OxOx)的催化作用。Ru@Pt-CNT/OxOx杂化电极的催化活性是仅含双金属复合材料电极的2.0倍。在计时安培实验中,混合电极的最大电流密度(2.65±0.15 mA cm-2)比Ru@Pt-CNT电极高35%。电化学阻抗谱分析表明,杂化电极的电荷转移电阻比Ru@Pt-CNT电极低,证实了OxOx在电极表面的生物电催化反应中对乳酸具有较高的亲和力。此外,通过长时间的体电解,发现在Ru@Pt-CNT/OxOx混合电极上的乳酸电氧化产生的总电荷为1.2±0.2 C,是Ru@Pt-CNT电极产生的总电荷的3倍。在本体电解过程中,通过色谱法检测了杂化电极产生的乳酸氧化产物,结果表明杂化生物膜从乳酸中获得了全部10个电子,并将其完全氧化为CO2。具有优异的稳定性和催化性能,混合电极在乳酸氧化的多个分解代谢步骤中起作用。总体而言,Ru@Pt-CNT和OxOx之间的相互作用增强了乳酸生物燃料电池的组装,从而改善了乳酸电氧化。这可能为开发在生物电化学中有前景的高效电子器件铺平道路。
Enhanced Biofuel Cells Based on a Hybrid Enzymatic/Bimetallic Composite for Complete Lactate Catalytic Electrooxidation.
We describe complete lactate electrooxidation in an enzymatic biofuel cell that combines the catalytic action of the bimetallic composite Ru@Pt-CNT and the enzyme oxalate oxidase (OxOx). The Ru@Pt-CNT/OxOx hybrid electrode was 2.0-fold more catalytically active than the electrode containing the bimetallic composite only. During chronoamperometric experiments, the hybrid electrode achieved a 35% higher maximum current density (2.65 ± 0.15 mA cm-2) than the Ru@Pt-CNT electrode. Electrochemical impedance spectroscopy showed that the hybrid electrode had lower charge transfer resistance than the Ru@Pt-CNT electrode, confirming that OxOx had a high affinity for lactate during the bioelectrocatalytic reaction on the electrode surface. Furthermore, 18-h long-term bulk electrolysis revealed that lactate electrooxidation at the Ru@Pt-CNT/OxOx hybrid electrode provided a total charge of 1.2 ± 0.2 C, which was 3-fold higher than the total charge generated by the Ru@Pt-CNT electrode. The lactate oxidation products generated at the hybrid electrode were detected during bulk electrolysis by chromatography, which showed that the hybrid biofilm harvested all 10 electrons from lactate, completely oxidizing it to CO2. With exceptional stability and catalytic performance, the hybrid electrode acted in the multiple catabolic steps of lactate oxidation. Overall, the interaction between Ru@Pt-CNT and OxOx enhanced the assembly of lactate biofuel cells to improve lactate electrooxidation. This could pave the way for developing efficient electronic devices with promising applications in bioelectrochemistry.
期刊介绍:
ACS Materials Au is an open access journal publishing letters articles reviews and perspectives describing high-quality research at the forefront of fundamental and applied research and at the interface between materials and other disciplines such as chemistry engineering and biology. Papers that showcase multidisciplinary and innovative materials research addressing global challenges are especially welcome. Areas of interest include but are not limited to:Design synthesis characterization and evaluation of forefront and emerging materialsUnderstanding structure property performance relationships and their underlying mechanismsDevelopment of materials for energy environmental biomedical electronic and catalytic applications