Preparation of Denitrification Materials with Nickel Slag for Nitric Oxide Decomposition in Cement Kilns.

NOx emission from the cement industry have received much attention. In order to reduce the NOx emission in cement kilns, nickel slag was used to prepare the non-ammonia denitrification material, and a denitrification mechanism was proposed in this study. The results showed that the denitrification material prepared at pH 7 exhibited the best denitrification performance. At low temperature, the highest denitrification performance was achieved between 200 and 300 °C with a NO decomposition rate of approximately 40%. Then, the NO decomposition rate increased as the temperature increased, reaching over 95% above 700 °C. The physicochemical characteristics showed that the material had the highest specific surface area and the highest relative Fe content, which benefited the denitrification performance. The divalent iron of the denitrification material was considered the active site for the reaction, and trivalent iron was not conducive to denitrification performance at a low temperature range. After the denitrification reaction, the Fe3+/Fe2+ increased from 0.89 to 1.31. The proposed denitrification mechanism was the redox process between divalent iron and trivalent iron. This study not only recycles industrial waste to reduce solid waste pollution but also efficiently removes nitrogen oxides from cement kilns without ammonia.

Tunable Interfacial Electronic Pd-Si Interaction Boosts Catalysis via Accelerating O2 and H2O Activation.

Engineering the interfacial structure between noble metals and oxides, particularly on the surface of non-reducible oxides, is a challenging yet promising approach to enhancing the performance of heterogeneous catalysts. The interface site can alter the electronic and d-band structure of the metal sites, facilitating the transition of energy levels between the reacting molecules and promoting the reaction to proceed in a favorable direction. Herein, we created an active Pd-Si interface with tunable electronic metal-support interaction (EMSI) by growing a thin permeable silica layer on a non-reducible oxide ZSM-5 surface (termed Pd@SiO2/ZSM-5). Our experimental results, combined with density functional theory calculations, revealed that the Pd-Si active interface enhanced the charge transfer from deposited Si to Pd, generating an electron-enriched Pd surface, which significantly lowered the activation barriers for O2 and H2O. The resulting reactive oxygen species, including O2 -, O2 2-, and -OH, synergistically facilitated formaldehyde oxidation. Additionally, moderate electronic metal-support interaction can promote the catalytic cycle of Pd0 ⇆ Pd2+, which is favorable for the adsorption and activation of reactants. This study provides a promising strategy for the design of high-performance noble metal catalysts for practical applications.

Boosting Ozone Catalytic Oxidation of Toluene at Room Temperature by Using Hydroxyl-Mediated MnOx/Al2O3 Catalysts.

Ozone catalytic oxidation (OZCO) has gained great interest in environmental remediation while it still faces a big challenge during the deep degradation of refractory volatile organic compounds (VOCs) at room temperature. Hydroxylation of the catalytic surface provides a new strategy for regulating the catalytic activity to boost VOC degradation. Herein, OZCO of toluene at room temperature over hydroxyl-mediated MnOx/Al2O3 catalysts was originally demonstrated. Specifically, a novel hydroxyl-mediated MnOx/Al2O3 catalyst was developed via the in situ AlOOH reconstruction method and used for toluene OZCO. The toluene degradation performance of MnOx/Al2O3 was significantly superior to those of most of the state-of-the-art catalysts, and 100% toluene was removed with an excellent mineralization rate (82.3%) and catalytic stability during OZCO. ESR and in situ DRIFTs results demonstrated that surface hydroxyl groups (HGs) greatly improved the reactive oxygen species generation, thus dramatically accelerating the benzene ring breakage and deep mineralization. Furthermore, HGs provided anchoring sites for uniformly dispersing MnOx and greatly enhanced toluene adsorption and ozone activation. This work paves a way for deep decomposition of aromatic VOCs at room temperature.

Exceptional Ozone Decomposition over δ-MnO2/AC under an Entire Humidity Environment.

Ozone (O3) pollution is highly detrimental to human health and the ecosystem due to it being ubiquitous in ambient air and industrial processes. Catalytic decomposition is the most efficient technology for O3 elimination, while the moisture-induced low stability represents the major challenge for its practical applications. Here, activated carbon (AC) supported δ-MnO2 (Mn/AC-A) was facilely synthesized via mild redox in an oxidizing atmosphere to obtain exceptional O3 decomposition capacity. The optimal 5Mn/AC-A achieved nearly 100% of O3 decomposition at a high space velocity (1200 L g-1 h-1) and remained extremely stable under entire humidity conditions. The functionalized AC provided well-designed protection sites to inhibit the accumulation of water on δ-MnO2. Density functional theory (DFT) calculations confirmed that the abundant oxygen vacancies and a low desorption energy of intermediate peroxide (O22-) can significantly boost O3 decomposition activity. Moreover, a kilo-scale 5Mn/AC-A with low cost (∼1.5 $/kg) was used for the O3 decomposition in practical applications, which could quickly decompose O3 pollution to a safety level below 100 µg m-3. This work offers a simple strategy for the development of moisture-resistant and inexpensive catalysts and greatly promotes the practical application of ambient O3 elimination.

Abatement of VOCs mixture of emerging concern by VUV-PCO process: From lab to pilot scale.

As a kind of emerging pollutant, volatile organic compounds (VOCs) are getting increasing attention due to their contribution to the formation of atmospheric haze and O3. Photocatalytic oxidation under vacuum ultraviolet photocatalytic oxidation (VUV-PCO) presents a promising method for VOCs degradation, but it is seldom studied for VOCs compound and the mechanism is still elusive. Herein, typical VOCs such as toluene and ethyl acetate were degraded separately or together in VUV system and in VUV-PCO system with the designed trifunctional catalyst Mn/TiO2/ZSM-5. Intermediates were recognized by PTR-TOF-MS. It is found that dual VOCs mixture outperformed single VOCs under both VUV process and VUV-PCO process. Possible degradation mechanisms were proposed. To explore the potential practicality of VUV-PCO technology, scale-up synthesis of Mn/TiO2/ZSM-5 on ceramic foams was successfully carried out and assembled into a homemade pilot-scale VUV-PCO equipment for the control of simulated VOCs complex (toluene, ethyl acetate, ethanol, and acetone). Pilot-scale catalytic testing with the monolithic catalysts achieved high removal efficiency (over 90 % efficiency after two cycles of regeneration) and confirmed the practical application possibility of VUV-PCO technology in multiple VOCs degradation. This work probes into the VUV-PCO technology applicability from lab scale to pilot scale and promotes the understanding of VUV and VUV-PCO in VOCs complex decomposition.

Facet-rotated echelle grating for cyclic wavelength router with uniform loss and flat passband.

A novel method for designing a cyclic echelle grating wavelength router with uniform loss and flat passband is proposed and experimentally demonstrated. A 4×4 cyclic wavelength router with a channel spacing of 400 GHz at 1550 nm wavelength band is designed and fabricated in InP. Measurement results show that the loss of 16 input-output combinations varies from 9 to 19.3 dB in a conventional design, with a nonuniformity of 10.3 dB, while the 1-dB spectral bandwidth is only 0.3 nm. By rotating angles of grating facets according to an appropriately designed distribution function, the loss nonuniformity is reduced to 1.5 dB, and a flat-top spectral response with 1 dB bandwidth of 1.0 nm is achieved simultaneously.