Alisson H.M. da Silva , Rafaël E. Vos , Robin J.C. Schrama , Marc T.M. Koper
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Additionally, online catalytic performance of CO<sub>2</sub> reduction to CO on a rotating polycrystalline gold disk electrode was investigated under different pressure and temperature. Our results indicate a positive impact of temperature on the faradaic efficiency (FE) towards CO up to 50 °C, beyond which a rapid drop in performance was observed at atmospheric pressure. Conversely, increasing pressure positively affected CO<sub>2</sub> solubility in the electrolyte, resulting in enhanced FE towards CO, reaching approximately 90 % at 6 bar compared to 40 % at atmospheric pressure. Notably, further increases in pressure did not significantly alter the FE, but led to higher current densities. Moreover, at pressures exceeding 6 bar, we observed a plateau in efficiency at temperatures higher than 50 °C. This observation suggests that increasing pressure can sustain CO<sub>2</sub> electrolysis, validating the hypothesis that increasing CO<sub>2</sub> solubility would suppress catalytic decay at higher temperatures. This study opens up promising avenues for future investigations in electrocatalysis, ranging from fundamental explorations of surface modifications induced by variations in temperature and pressure to the development of high-performance catalysts.</p></div>","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":null,"pages":null},"PeriodicalIF":5.5000,"publicationDate":"2024-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0013468624008521/pdfft?md5=44438241ab6cbe6a2d1d38b941ad0d57&pid=1-s2.0-S0013468624008521-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Design of a Rotating Disk Electrode setup operating under high pressure and temperature: Application to CO2 reduction on gold\",\"authors\":\"Alisson H.M. da Silva , Rafaël E. Vos , Robin J.C. Schrama , Marc T.M. 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Our results indicate a positive impact of temperature on the faradaic efficiency (FE) towards CO up to 50 °C, beyond which a rapid drop in performance was observed at atmospheric pressure. Conversely, increasing pressure positively affected CO<sub>2</sub> solubility in the electrolyte, resulting in enhanced FE towards CO, reaching approximately 90 % at 6 bar compared to 40 % at atmospheric pressure. Notably, further increases in pressure did not significantly alter the FE, but led to higher current densities. Moreover, at pressures exceeding 6 bar, we observed a plateau in efficiency at temperatures higher than 50 °C. This observation suggests that increasing pressure can sustain CO<sub>2</sub> electrolysis, validating the hypothesis that increasing CO<sub>2</sub> solubility would suppress catalytic decay at higher temperatures. 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引用次数: 0
摘要
我们介绍了旋转盘电极(RDE)电池的设计与开发,该电池能够在压力高达 200 巴、温度高达 200 ℃ 的条件下工作。这种装置可以在不同的质量传输条件下,通过伏安法和阻抗光谱法等技术进行电化学表面表征。此外,由于该系统以半连续模式工作,并与在线气体样品测量相连接,因此可以对催化性能(包括二氧化碳还原)进行评估。为了验证所设计的高压电池的概念,我们研究了多晶金在高达 150 °C 和 50 bar 的温度条件下循环伏安图(CV)随温度的变化。此外,我们还研究了旋转多晶金盘电极在不同压力和温度下将 CO2 还原成 CO 的在线催化性能。我们的研究结果表明,温度对一氧化碳的法拉第效率(FE)有积极影响,最高可达 50 °C,超过 50 °C,在常压下性能会迅速下降。相反,压力的增加会对电解液中的二氧化碳溶解度产生积极影响,从而提高对一氧化碳的远动效率,在 6 巴压力下达到约 90%,而在常压下仅为 40%。值得注意的是,进一步增加压力并不会显著改变 FE,但会导致更高的电流密度。此外,当压力超过 6 巴时,我们观察到在温度高于 50 °C时效率会达到一个平稳点。这一观察结果表明,增加压力可以维持二氧化碳电解,从而验证了增加二氧化碳溶解度可抑制高温下催化衰减的假设。这项研究为未来的电催化研究开辟了广阔的前景,从温度和压力变化引起的表面改性的基础探索到高性能催化剂的开发,不一而足。
Design of a Rotating Disk Electrode setup operating under high pressure and temperature: Application to CO2 reduction on gold
We describe the design and development of a rotating disk electrode (RDE) cell capable of operating at pressures up to 200 bar and temperatures up to 200 °C. This setup enables electrochemical surface characterization through techniques such as voltammetry and impedance spectroscopy, under different mass transport regimes. Furthermore, evaluation of catalytic performance, including CO2 reduction, is possible as the system works in a semi-continuous mode interfaced with online gas sample measurements. As a proof of concept of the high-pressure cell designed, we examined the temperature-dependent changes in the cyclic voltammograms (CVs) of polycrystalline gold up to 150 °C and 50 bar. Additionally, online catalytic performance of CO2 reduction to CO on a rotating polycrystalline gold disk electrode was investigated under different pressure and temperature. Our results indicate a positive impact of temperature on the faradaic efficiency (FE) towards CO up to 50 °C, beyond which a rapid drop in performance was observed at atmospheric pressure. Conversely, increasing pressure positively affected CO2 solubility in the electrolyte, resulting in enhanced FE towards CO, reaching approximately 90 % at 6 bar compared to 40 % at atmospheric pressure. Notably, further increases in pressure did not significantly alter the FE, but led to higher current densities. Moreover, at pressures exceeding 6 bar, we observed a plateau in efficiency at temperatures higher than 50 °C. This observation suggests that increasing pressure can sustain CO2 electrolysis, validating the hypothesis that increasing CO2 solubility would suppress catalytic decay at higher temperatures. This study opens up promising avenues for future investigations in electrocatalysis, ranging from fundamental explorations of surface modifications induced by variations in temperature and pressure to the development of high-performance catalysts.
期刊介绍:
Electrochimica Acta is an international journal. It is intended for the publication of both original work and reviews in the field of electrochemistry. Electrochemistry should be interpreted to mean any of the research fields covered by the Divisions of the International Society of Electrochemistry listed below, as well as emerging scientific domains covered by ISE New Topics Committee.