Search

Catalytic oxidation technology is a promising strategy to eliminate carbon monoxide (CO), volatile organic compounds (VOC) and other emissions from industrial boilers and to address ammonia (NH 3) escape. Herein, we demonstrate the potential of copper-cerium-zirconium mixed oxides or those supported on TiO 2 or ZSM-5 substrates for the simultaneous catalytic removal of CO, toluene and NH 3. Among them, CuCeZr/ZSM-5 exhibits the best co-processing ability for mixed gases. In situ infrared spectroscopy analyses suggest that there is a competitive adsorption among CO, toluene and NH 3 , and the inhibition is in descending order of toluene＞CO＞NH 3. Based on the physical-chemical characterizations, the Cu-Ce interfacial structure plays an important role in CO ignition at low temperatures. More importantly, the abundant acidic sites on the ZSM-5 support can improve the stability of adsorbed NH 3 at high temperatures, resulting in the best NH 3 catalytic oxidation performance of CuCeZr/ZSM-5 with no secondary pollutants of NO x. This study provides a strategy for the catalyst design to eliminate multiple pollutants targeting the properties of pollutants. [Display omitted] • Simultaneous removal of CO, toluene and NH 3 was achieved by CuCeZr based catalyst. • The best mixed gas treatment was observed for CuCeZr/ZSM-5 catalyst. • Cu-Ce interfacial structure allows preferential ignition of CO at low temperature. • The acidic sites on the ZSM-5 promoted the adsorption and oxidation of NH 3. [ABSTRACT FROM AUTHOR]

CO self-sustaining catalytic combustion tends to be one of potential means to achieve efficient conversion of off-gases from steelmaking. Building model catalysts to investigate the reaction process academically is essential to design optimized catalysts and Cu 2 O exposing (1 0 0), (1 1 1) and (1 1 0) planes are excellent materials. Herein, morphological CeO 2 /Cu 2 O inverse model catalysts were synthesized to reveal the synergistic effect and reaction mechanism. It is demonstrated that the ignition temperature is lowered on the interface by synergistic effect, which dominates the ignition, while the combustion after ignition is controlled by Cu 2 O planes providing abundant lattice oxygen to react with CO. Additionally, exposure of different planes plays a significant role in the reaction since O-termination on (1 0 0) inhibits the interaction, whereas Cu-termination on (1 1 0) surface structure and coordinately unsaturated Cu+ on open (1 1 1) surface respectively contribute to their superior catalytic performance. [Display omitted] ● Inverse model CeO 2 /Cu 2 O catalysts with regular morphology were successfully prepared. ● Synergistic effect on Cu-Ce interface lowered ignition temperature, dominating the ignition. ● The catalytic activity and synergistic effect vary among planes with (1 1 1) performing the best. ● Exposure of crystal planes with higher activity assists in designing optimized catalysts. [ABSTRACT FROM AUTHOR]

Cubic Cu 2 O micro/nanocrystals were successfully synthesized by liquid-phase reduction using copper salt of CuSO 4 or CuCl 2 ·2H 2 O, and glucose or ascorbic acid as reducing agent, respectively. The activity of the catalysts was evaluated by light-off curves of CO self-sustained catalytic combustion via temperature-programmed oxidation of CO (CO-TPO), with the results showing the activity of catalysts following the order of Cu 2 O–Cl-GLU > Cu 2 O– S -GLU > Cu 2 O– S -AA > Cu 2 O–Cl-AA, (Cl denotes CuCl 2 ·2H 2 O, GLU denotes glucose, S denotes CuSO 4 and AA denotes ascorbic acid, respectively), corresponding to the ignition temperature of 109 °C, 122 °C, 137 °C and 186 °C, respectively. The crystal structure, elemental valence, morphology and redox property of the prepared catalysts were analyzed by using various characterization techniques. Combined with in situ infrared spectrum, the CO self-sustained catalytic combustion over Cu 2 O catalysts mainly follows the Mars-van-Krevelen (M-v-K) mechanism: the adsorbed and activated CO reacts with lattice oxygen to yield CO 2 and oxygen vacancy, and then the oxygen vacancy can be replenished by gaseous oxygen. Combined with catalytic performance of high-concentration CO, it is found that the catalysts prepared using glucose as reducing agent are more angular compared with ascorbic acid. The Cu 2 O–Cl-GLU synthesized with glucose and CuCl 2 ·2H 2 O exhibits the best catalytic activity among all the catalysts tested, attributing to its more obvious edge and rough crystal surface. The unique structure of Cu 2 O–Cl-GLU leads to the high exposure rate and coordination unsaturation of atoms on the cubic Cu 2 O micro/nanocrystals that can improve the ability of activating gaseous O 2 and low temperature reducibility, and consequently facilitating the catalytic activity. Cycle path diagram of CO oxidation reaction (a) and schematic diagram of CO oxidation reaction on Cu 2 O (b). [Display omitted] • Effects of reducing agent on catalytic properties is greater than that of copper salt. • High concentration CO can achieve self-sustained catalytic combustion on obtained Cu 2 O. • Glucose enhances unsaturation of Cu atoms contributing to high activity. • Chemically adsorbed oxygen on Cu 2 O surface promotes CO ignition. [ABSTRACT FROM AUTHOR]