The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of...The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H_(2)O are adsorbed and activated by oxygen vacancy.The 10 at%Cu doped Co_(3)O_(4) sample(10Cu-Co_(3)O_(4))exhibits the optimal activity,100%of COS conversion at 70℃.The improved oxygen vacancies of CueCo_(3)O_(4) accelerate the activation of H_(2)O to form active -OH.COS binds with hydroxyl to form the intermediate HSCO^(-)_(2),and then the activated-OH on the oxygen vacancy reacts with HSCO^(-)_(2) to form HCO^(-)_(3).Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu^(2+))redox cycle mitigate the sulfation of Co_(3)O_(4)(Co^(2+)/Co^(3+)).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.展开更多
Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^...Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^(-1), while the removal performance of H_2S withcatalysts was investigated using the thermal gravimetric method. The results show that the catalystsare highly active for COS hydrolysis at low temperatures (≤60 ℃) and high gas hourly spacevelocity, and the highest activity can reach 100%. The catalyst is particularly stable for 12 h, andno deactivation is observed. Nanoparticle α-FeOOH prepared using hydrated iron sulfate showshigher COS hydrolysis activity, and the optimum calcination temperature for the catalyst is 260 ℃.In addition, the catalysts can remove COS and H_2S simultaneously, and 60 ℃ is favorable for theremoval of H_2S. The compensation effect exists in nanoparticle-based catalysts.展开更多
基金the National Natural Science Foundation of China (92034301,22078063 and 22022804)Major Program of Qingyuan Innovation Laboratory (00121003)the Natural Science Foundation of Fujian Province (2020H6007)。
文摘The activation of H_(2)O is a key step of the COS hydrolysis,which may be tuned by oxygen vacancy defects in the catalysts.Herein,we have introduced Cu into Co_(3)O_(4) to regulate the oxygen vacancy defect content of the catalysts.In situ DRIFTS and XPS spectra reveal that COS and H_(2)O are adsorbed and activated by oxygen vacancy.The 10 at%Cu doped Co_(3)O_(4) sample(10Cu-Co_(3)O_(4))exhibits the optimal activity,100%of COS conversion at 70℃.The improved oxygen vacancies of CueCo_(3)O_(4) accelerate the activation of H_(2)O to form active -OH.COS binds with hydroxyl to form the intermediate HSCO^(-)_(2),and then the activated-OH on the oxygen vacancy reacts with HSCO^(-)_(2) to form HCO^(-)_(3).Meanwhile,the catalyst exhibits high catalytic stability because copper species(Cu+/Cu^(2+))redox cycle mitigate the sulfation of Co_(3)O_(4)(Co^(2+)/Co^(3+)).Our work offers a promising approach for the rational design of cobalt-related catalysts in the highly efficient hydrolysis COS process.
文摘Catalysts using α-FeOOH nanoparticles as the active ingredient were testedby a microreactor-chromatography assessing apparatus at atmospheric pressure between 25 and 60 ℃with a gas hourly space velocity of 10,000 h^(-1), while the removal performance of H_2S withcatalysts was investigated using the thermal gravimetric method. The results show that the catalystsare highly active for COS hydrolysis at low temperatures (≤60 ℃) and high gas hourly spacevelocity, and the highest activity can reach 100%. The catalyst is particularly stable for 12 h, andno deactivation is observed. Nanoparticle α-FeOOH prepared using hydrated iron sulfate showshigher COS hydrolysis activity, and the optimum calcination temperature for the catalyst is 260 ℃.In addition, the catalysts can remove COS and H_2S simultaneously, and 60 ℃ is favorable for theremoval of H_2S. The compensation effect exists in nanoparticle-based catalysts.
