Formaldehyde(HCHO) and carbon monoxide(CO) are both common air pollutants and hazardous to human body. It is imperative to develop the catalyst that is able to efficiently remove these pollutants. In this work, we act...Formaldehyde(HCHO) and carbon monoxide(CO) are both common air pollutants and hazardous to human body. It is imperative to develop the catalyst that is able to efficiently remove these pollutants. In this work, we activated Pt-MnO_(2)under different conditions for highly active oxidation of HCHO and CO, and the catalyst activated under CO displayed superior performance. A suite of complementary characterizations revealed that the catalyst activated with CO created the highly dispersed Pt nanoparticles to maintain a more positively charged state of Pt, which appropriately weakens the Mn-O bonding strength in the adjacent region of Pt for efficient supply of active oxygen during the reaction. Compared with other catalysts activated under different conditions, the CO-activated Pt-MnO_(2)displays much higher activity for oxidation of HCHO and CO. This research contributes to elucidating the mechanism for regulating the oxidation activity of Pt-based catalyst.展开更多
While supported-noble-metal catalysts have been widely investigated in hydrotreating reactions,a crucial issue that the catalytic system is still confronted with is developing an efficient approach to gain the high di...While supported-noble-metal catalysts have been widely investigated in hydrotreating reactions,a crucial issue that the catalytic system is still confronted with is developing an efficient approach to gain the high dispersion of noble metals under reducing conditions.In this work,Ru was supported on two MnOx with different specific surface areas(SSAs),and a much higher dispersion of Ru(83%,in contrast to 42%of the other one)was surprisingly observed over MnO with much lower SSA(around one-third of the other one).A suite of complementary characterizations demonstrates that,compared with the catalyst with high SSA(Ru/MnO-H),the MnO in the one with lower SSA(Ru/MnO-L)contains enriched surface oxygen that creates more abundant sites and bears stronger strength to anchor Ru species,mitigating the aggregation of Ru under reducing condition.This not only enriched active sites(i.e.,exposed Ru),but also created a more electron-deficient Ru domain and thus enhanced the redox property of the surface,leading to the lower barrier for C–O bond hydrogenolysis.In the hydrogenolysis of diphenyl ether,Ru/MnO-L exhibited significantly enhanced activity(i.e.,6 folds of Ru/MnO-H)and high stability.This work provides an approach to regulate the surface chemistry of support for the high dispersion of supported metal.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 22025604, 21976196, 21972170 and 22072184)。
文摘Formaldehyde(HCHO) and carbon monoxide(CO) are both common air pollutants and hazardous to human body. It is imperative to develop the catalyst that is able to efficiently remove these pollutants. In this work, we activated Pt-MnO_(2)under different conditions for highly active oxidation of HCHO and CO, and the catalyst activated under CO displayed superior performance. A suite of complementary characterizations revealed that the catalyst activated with CO created the highly dispersed Pt nanoparticles to maintain a more positively charged state of Pt, which appropriately weakens the Mn-O bonding strength in the adjacent region of Pt for efficient supply of active oxygen during the reaction. Compared with other catalysts activated under different conditions, the CO-activated Pt-MnO_(2)displays much higher activity for oxidation of HCHO and CO. This research contributes to elucidating the mechanism for regulating the oxidation activity of Pt-based catalyst.
基金the National Natural Science Foundation of China(Nos.22025604,21976196,21936005,and 21878244)the fellowship of China Postdoctoral Science Foundation(No.2022M713308)the Special Project of Eco-environmental Technology for Emission Peak&Carbon Neutralization(No.RCEES-TDZ-2021-4).
文摘While supported-noble-metal catalysts have been widely investigated in hydrotreating reactions,a crucial issue that the catalytic system is still confronted with is developing an efficient approach to gain the high dispersion of noble metals under reducing conditions.In this work,Ru was supported on two MnOx with different specific surface areas(SSAs),and a much higher dispersion of Ru(83%,in contrast to 42%of the other one)was surprisingly observed over MnO with much lower SSA(around one-third of the other one).A suite of complementary characterizations demonstrates that,compared with the catalyst with high SSA(Ru/MnO-H),the MnO in the one with lower SSA(Ru/MnO-L)contains enriched surface oxygen that creates more abundant sites and bears stronger strength to anchor Ru species,mitigating the aggregation of Ru under reducing condition.This not only enriched active sites(i.e.,exposed Ru),but also created a more electron-deficient Ru domain and thus enhanced the redox property of the surface,leading to the lower barrier for C–O bond hydrogenolysis.In the hydrogenolysis of diphenyl ether,Ru/MnO-L exhibited significantly enhanced activity(i.e.,6 folds of Ru/MnO-H)and high stability.This work provides an approach to regulate the surface chemistry of support for the high dispersion of supported metal.
