Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water techniq...Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.展开更多
合理的设计策略以提高贵金属电催化剂在析氢反应(HER)中的利用率,对于简化HER的工艺流程,促进未来能源循环经济的发展至关重要.本文在约2.4 nm的Ru纳米颗粒上设计了大量的缺陷,使其在苛刻的酸性和碱性电解质中具有超高质量比反应活性....合理的设计策略以提高贵金属电催化剂在析氢反应(HER)中的利用率,对于简化HER的工艺流程,促进未来能源循环经济的发展至关重要.本文在约2.4 nm的Ru纳米颗粒上设计了大量的缺陷,使其在苛刻的酸性和碱性电解质中具有超高质量比反应活性.在过电势为100 m V时,所制备的缺陷富集型Ru基电催化剂DR-Ru表现出超高的HER翻转频率(碱性:16.4 s^(-1);酸性:20.6 s^(-1))和超低的过电势(碱性:η10=28.2 m V;酸性:η10=25.1 mV),明显优于其他Ru基电催化剂.此外,低配位的Ru活性位和表面部分晶格氧削弱了DR-Ru的Ru–H结合能,促进了酸性HER进行;同时有利于H2O分子分解,缓解了碱性HER过程中水分子的解离迟滞,导致其具有与酸性HER相当的高质量比活性.展开更多
A comprehensive understanding of the microscopic reaction mechanisms at the gas-solid-liquid electrochemical interfaces is urgently required for the development of advanced electrocatalysts applied in burgeoning susta...A comprehensive understanding of the microscopic reaction mechanisms at the gas-solid-liquid electrochemical interfaces is urgently required for the development of advanced electrocatalysts applied in burgeoning sustainable energy conversion systems. In-situ synchrotron radiation Fourier transform infrared(SR-FTIR) spectroscopy is one of the most powerful techniques for investigating the evolving dynamics of reactive intermediates during electrocatalytic reactions. In this review, we methodically summarize the recent progress in the research of dynamic mechanisms for valuable electrocatalytic reactions based on in-situ SR-FTIR methodology. Moreover, the merits and drawbacks of SRFTIR spectroscopy, the design principles of infrared beam setups and in-situ cells, as well as the in-situ measurement criteria are also discussed in detail. Lastly, the potential challenges and opportunities in this field are prudently stated. This review is expected to stimulate a broad interest in the material science and electrochemistry communities for exploring the dynamic mechanisms of prominent catalysis at the atomic/molecular level by using SR-based spectroscopy.展开更多
基金supported by the National Natural Science Foundation of China(12205300 and 12135012)the Natural Science Foundation of Anhui Province(2208085QA28 and 2208085J01)。
文摘Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.
基金supported by the National Natural Science Foundation of China (U1932212, 11875257, and U1932109)the Fundamental Research Funds for the Central Universities (WK2310000070)
文摘合理的设计策略以提高贵金属电催化剂在析氢反应(HER)中的利用率,对于简化HER的工艺流程,促进未来能源循环经济的发展至关重要.本文在约2.4 nm的Ru纳米颗粒上设计了大量的缺陷,使其在苛刻的酸性和碱性电解质中具有超高质量比反应活性.在过电势为100 m V时,所制备的缺陷富集型Ru基电催化剂DR-Ru表现出超高的HER翻转频率(碱性:16.4 s^(-1);酸性:20.6 s^(-1))和超低的过电势(碱性:η10=28.2 m V;酸性:η10=25.1 mV),明显优于其他Ru基电催化剂.此外,低配位的Ru活性位和表面部分晶格氧削弱了DR-Ru的Ru–H结合能,促进了酸性HER进行;同时有利于H2O分子分解,缓解了碱性HER过程中水分子的解离迟滞,导致其具有与酸性HER相当的高质量比活性.
基金supported by the National Natural Science Foundation of China (Nos. 1932212, U1932109, 11875257)。
文摘A comprehensive understanding of the microscopic reaction mechanisms at the gas-solid-liquid electrochemical interfaces is urgently required for the development of advanced electrocatalysts applied in burgeoning sustainable energy conversion systems. In-situ synchrotron radiation Fourier transform infrared(SR-FTIR) spectroscopy is one of the most powerful techniques for investigating the evolving dynamics of reactive intermediates during electrocatalytic reactions. In this review, we methodically summarize the recent progress in the research of dynamic mechanisms for valuable electrocatalytic reactions based on in-situ SR-FTIR methodology. Moreover, the merits and drawbacks of SRFTIR spectroscopy, the design principles of infrared beam setups and in-situ cells, as well as the in-situ measurement criteria are also discussed in detail. Lastly, the potential challenges and opportunities in this field are prudently stated. This review is expected to stimulate a broad interest in the material science and electrochemistry communities for exploring the dynamic mechanisms of prominent catalysis at the atomic/molecular level by using SR-based spectroscopy.
