Rationally engineered ReO -CuSO4/TiO2 catalyst with superior NH3-SCO efficiency and remarkably boosted SO2 tolerance: Synergy of acid sites and surface adsorbed oxygen

Yu, Yanke; Wei, Desheng; Tong, Zhaojian; Wang, Jinxiu; Chen, Jinsheng; He, Chi

doi:10.1016/j.cej.2022.136356

Cited by 39 publications

(26 citation statements)

References 47 publications

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“…The band at 1386 cm −1 could be associated with -NH2 wagging. Two bands at 1270 and 1601 cm −1 were the typical bands of NH3 adsorbed on Lewis (L) acid sites 33 . The band at 1442 cm −1 and the broad band (1650-1800 cm −1 ) could be associated with chemisorbed NH4 + on Brønsted (B) acid sites 32 .…”

Section: Surface Reducibility and Aciditymentioning

confidence: 99%

Effect of Potassium on the Performance of a CuSO4/TiO2 Catalyst Used in the Selective Catalytic Reduction of NOx by NH3

Yu¹,

Geng²,

Wei³

et al. 2022

Acta Physico Chimica Sinica

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Owing to its renewability, abundance, and low environmental impact, biomass is considered to be a viable eco-friendly fuel. Various biofuelfired power plants have been built worldwide to reduce carbon emissions. Potassium (K) is a typical impurity in the flue gas from biofuel combustion that can deactivate the catalyst used in the selective catalytic reduction of NOx by ammonia (NH3-SCR). CuSO4/TiO2, with excellent sulfur dioxide tolerance, is thought to be a promising vanadium-free catalyst for NH3-SCR; however, the influence of K on the CuSO4/TiO2 catalyst is still unknown. Therefore, in this study, the effect of K on the NH3-SCR performance of CuSO4/TiO2 were investigated and compared with the effect on the performance of the commercial V2O5-WO3/TiO2 (VWTi) catalyst. K-poisoned catalysts were prepared via wet impregnation using potassium acetate as the K source. Nitrogen (N2) adsorption-desorption, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), NH3-temperature programmed desorption (NH3-TPD), H2temperature programmed reduction (H2-TPR), and in situ diffuse reflectance infrared Fourier-transform spectroscopy (in situ DRIFTS) were used to characterize the prepared catalysts. The NOx conversion over CuSO4/TiO2 with 1.0% (w) K was 92.1% (at 350 °C), which was higher than the conversion (75.1%) achieved over the commercial VWTi catalyst with the same K content. The XRD, XPS, and H2-TPR results suggested that K reacted with the CuSO4 in the CuSO4/TiO2 catalyst to form CuO and K2SO4. The presence of CuO enhanced the oxidation of NH3 to N2O, NO, and NO2 during NH3-SCR, thereby decreasing the NOx conversion and N2 selectivity over CuSO4/TiO2. Moreover, based on the results from NH3-TPD and in situ DRIFTS of NH3 adsorption, it can be concluded that the Brønsted acid sites (S-OH) were poisoned by K, which restrained the adsorption of NH3 on CuSO4/TiO2. Additionally, the high K content altered the pore structure of the catalyst, leading to a decrease in the specific surface area. However, according to the in situ DRIFTS results, NH3-SCR over K-poisoned CuSO4/TiO2 still followed the Eley-Rideal mechanism: First, NH3 was adsorbed on the Lewis and Brønsted acid sites of the catalyst, and then gaseous NO and O2 reacted with the adsorbed NH3/NH4+ on the acid sites, resulting in the formation of N2 and H2O. Notably, the abundance of acid sites and surface-adsorbed oxygen species on CuSO4/TiO2 could be the main reason for its higher resistance to K-poisoning. In conclusion, our current findings suggested that CuSO4/TiO2 might be a suitable NH3-SCR catalyst for use in the flue gas streams from biofuel-fired power plants.

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Section: Surface Reducibility and Aciditymentioning

confidence: 99%

Effect of Potassium on the Performance of a CuSO4/TiO2 Catalyst Used in the Selective Catalytic Reduction of NOx by NH3

Yu¹,

Geng²,

Wei³

et al. 2022

Acta Physico Chimica Sinica

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“…In Fig. 7(b), for Mn/Zr-MCM-41, two peaks at B1472 and B1658 cm À1 are due to the NH 4 + species adsorbed on the Brønsted acid (B-acid) sites, 47,48 and the peak at B1619 cm À1 is the coordinated NH 3 adsorbed on the L-acid sites. This observation suggests that introduction of Zr results in the presence of B-acid sites and more abundant L-acid sites on the catalyst surface.…”

Section: Surface Aciditymentioning

confidence: 99%

A comparative study of Zr, Al or Sr doped Mn/MCM-41 for NH₃-SCR and resistance to SO₂/H₂O

Guo

et al. 2022

New J. Chem.

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“…Commercially available vanadiumbased catalysts have been reported to be suitable for the NH 3 -SCR process owing to the presence of V 5+ ; however, the oxidation of NH 3 remains limited [24]. Copper-based catalysts have generally been studied as NH 3 -SCO catalysts with excellent catalytic properties, such as high N 2 selectivity and relatively low costs [25][26][27][28][29][30]. In particular, NO X conversion efficiencies of 90% at 350 • C have been reported for the Cu/Ti catalysts, which uses TiO 2 as a support [31].…”

Section: Introductionmentioning

confidence: 99%

High-Dispersed V2O5-CuOX Nanoparticles on h-BN in NH3-SCR and NH3-SCO Performance

Lee

Kim

et al. 2022

Nanomaterials

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Typically, to meet emission regulations, the selective catalytic reduction of NOX with NH3 (NH3-SCR) technology cause NH3 emissions owing to high NH3/NOX ratios to meet emission regulations. In this study, V-Cu/BN-Ti was used to remove residual NOX and NH3. Catalysts were evaluated for selective catalytic oxidation of NH3 (NH3-SCO) in the NH3-SCR reaction at 200–300 °C. The addition of vanadium and copper increased the number of Brønsted and Lewis acid sites available for the reaction by increasing the ratio of V5+ and forming Cu+ species, respectively. Furthermore, h-BN was dispersed in the catalyst to improve the content of vanadium and copper species on the surface. NH3 and NOX conversion were 98% and 91% at 260 °C, respectively. Consequently, slipped NH3 (NH3-Slip) emitted only 2% of the injected ammonia. Under SO2 conditions, based on the NH3 oxidation reaction, catalytic deactivation was improved by addition of h-BN. This study suggests that h-BN is a potential catalyst that can help remove residual NOX and meet NH3 emission regulations when placed at the bottom of the SCR catalyst layer in coal-fired power plants.

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Rationally engineered ReO -CuSO4/TiO2 catalyst with superior NH3-SCO efficiency and remarkably boosted SO2 tolerance: Synergy of acid sites and surface adsorbed oxygen

Cited by 39 publications

References 47 publications

Effect of Potassium on the Performance of a CuSO<sub>4</sub>/TiO<sub>2</sub> Catalyst Used in the Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub>

Effect of Potassium on the Performance of a CuSO<sub>4</sub>/TiO<sub>2</sub> Catalyst Used in the Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub>

A comparative study of Zr, Al or Sr doped Mn/MCM-41 for NH₃-SCR and resistance to SO₂/H₂O

High-Dispersed V2O5-CuOX Nanoparticles on h-BN in NH3-SCR and NH3-SCO Performance

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Rationally engineered ReO -CuSO4/TiO2 catalyst with superior NH3-SCO efficiency and remarkably boosted SO2 tolerance: Synergy of acid sites and surface adsorbed oxygen

Cited by 39 publications

References 47 publications

Effect of Potassium on the Performance of a CuSO<sub>4</sub>/TiO<sub>2</sub> Catalyst Used in the Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub>

Effect of Potassium on the Performance of a CuSO<sub>4</sub>/TiO<sub>2</sub> Catalyst Used in the Selective Catalytic Reduction of NO<sub><i>x</i></sub> by NH<sub>3</sub>

A comparative study of Zr, Al or Sr doped Mn/MCM-41 for NH3-SCR and resistance to SO2/H2O

High-Dispersed V2O5-CuOX Nanoparticles on h-BN in NH3-SCR and NH3-SCO Performance

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A comparative study of Zr, Al or Sr doped Mn/MCM-41 for NH₃-SCR and resistance to SO₂/H₂O