Showing papers by "Changbin Zhang published in 2012"

Alkali‐Metal‐Promoted Pt/TiO2 Opens a More Efficient Pathway to Formaldehyde Oxidation at Ambient Temperatures

Abstract: Formaldehyde is emitted from building and furnishing materials and consumer products, and is known to cause irritation of eyes and respiratory tract, headache, pneumonia, and even cancer. It is a dominant indoor air pollutant, especially in developing countries, and significant efforts have gone into indoor HCHO purification to meet environmental regulations and human health needs. Removal of HCHO by adsorbents has been investigated extensively using potassium permanganate, activated carbon, aluminum oxide, and some ceramic materials. Sorbent effectiveness is typically limited by low adsorption capacities. Catalytic oxidation is the most effective technology for volatile organic compound (VOC) abatement because VOCs can be oxidized to CO2 over certain catalysts at much lower temperatures than in thermal oxidation. Supported noble metal catalysts (Pt, Pd, Rh, Au, Ag) or metal oxide catalysts (Ni, Cu, Cr, Mn) have been used for the catalytic oxidation of VOCs. Complete oxidation of HCHO over catalysts occurs above 150 8C on clean and oxidized films of Ni, Pd, and Al and over silver–cerium composite oxide, above 100 8C over Ag/MnOx-CeO2 [18] and Au/CeO2, [19] and above 85 8C over Pd-Mn/Al2O3 [17] and Au/FeOx. As catalytic oxidation at even lower temperatures is desirable for indoor air purification, the development of a catalyst for total HCHOoxidation at room temperature is of great interest. In our recent study, 1% Pt/TiO2 catalyst was shown to be effective for HCHO oxidation at room temperature, achieving 100% conversion of d= 100 ppm HCHO to CO2 and H2O at a gas hourly space velocity (GHSV) of 50000 h . However, we also observed that this type catalyst is not as active as needed for practical applications, and deactivates with time-on-stream. Herein, we report a novel alkali-metal-promoted Pt/TiO2 catalyst for the ambient destruction of HCHO. We show that the addition of alkali-metal ions (such as Li, Na, and K) to Pt/TiO2 catalyst stabilized an atomically dispersed PtO(OH)x–alkali-metal species on the catalyst surface and also opened a new low-temperature reaction pathway, significantly promoting the activity for the HCHO oxidation by activating H2O and catalyzing the facile reaction between surface OH and formate species to total oxidation products. Figure 1a shows the HCHO conversion to CO2 as a function of temperature over the x% Na-1% Pt/TiO2 (x= 0, 1, and 2) samples at a GHSVof 120000 h 1 andHCHO inlet of d= 600 ppm. All gas streams were humidified to a RH of around 50%. Before each activity test, the samples were reduced in H2 at 300 8C for 30 min. The sodium-free catalyst had low activity for the HCHO oxidation reaction, with HCHO conversion being only about 19% at 15 8C. With 1% Na addition, the HCHO conversion reached 96% at 15 8C and 100% at 40 8C. With 2% Na addition, 100% HCHO conversion to CO2 and H2O was measured at 15 8C. The effect of Na addition on the surface reducibility was examined by H2 temperature-programmed reduction (TPR; Figure 1b). The amounts of H2 consumption were about the same over all the samples, but the addition of Na shifted the reduction peak to lower temperatures, that is, from 2 8C for 1% Pt/TiO2 to 6 8C for 1% Na-1% Pt/TiO2 and 11 8C for 2% Na-1% Pt/ TiO2. Thus, the sample reducibility correlates with the sample activity. The most active 2% Na-promoted sample had excellent stability as checked by long isothermal tests. For example, at a GHSV of 300000 h 1 and with the same other reaction conditions, approximately 80% HCHO conversion was maintained over a 72 h-long test (Figure 1a, inset). Li and K were equally effective promoters to Na and imparted the same high activity and stability to the Pt species (Supporting Information, Figure S1). Water vapor and oxygen effects on the activity of Na-Pt/TiO2 are important (Supporting Information, Figures S2,S3). Deionized-water washing of the samples was performed to check the alkali-metal and Pt interaction.While most of the Na was removed from the Nacontaining catalysts, a residual amount remained (Supporting Information, Table S1). Activity test results (Supporting Information, Figure S1) showed that the washed catalyst had identical activity for HCHO [*] C. Zhang, F. Liu, Y. Liu, Prof. H. He Research Center for Eco-Environmental Sciences Chinese Academy of Sciences Shuangqing Road 18, Beijing, 100085 (China) E-mail: honghe@rcees.ac.cn

A superior Ce-W-Ti mixed oxide catalyst for the selective catalytic reduction of NOx with NH3

Abstract: A superior Ce-W-Ti mixed oxide catalyst prepared by a facile homogeneous precipitation method showed excellent NH3-SCR activity and 100% N2 selectivity with broad operation temperature window and extremely high resistance to space velocity, which is a very promising catalyst for NOx abatement from diesel engine exhaust. The excellent catalytic performance is associated with the highly dispersed active Ce and promotive W species on TiO2. The introduction of W species could increase the amount of active sites, oxygen vacancies, and Bronsted and Lewis acid sites over the catalyst, which is also beneficial to improve the low temperature activity by facilitating “fast SCR” reaction and enhance both of the high temperature activity and N2 selectivity simultaneously by inhibiting the unselective oxidation of NH3 at high temperatures.

Glucose production from hydrolysis of cellulose over a novel silica catalyst under hydrothermal conditions.

Abstract: A novel silica catalyst was synthesized by evaporation-induced self-assembly (EISA) method and tested for the catalytic selective hydrolysis of cellulose to glucose. This silica catalyst exhibited a higher catalytic activity than other oxides prepared by the same method, such as ZrO2, TiO2, and Al2O3. Using silica as a catalyst, cellulose was selectively hydrolyzed into glucose with a glucose yield as high as 50% under hydrothermal conditions without hydrogen gas. The silica catalyst was characterized by Brunauer-Emmett-Teller (BET), X-ray diffraction (XRD) and transmission electron microscopy (TEM). The results of temperature-programmed desorption of ammonia (NH3-TPD) and textural properties indicated that the synergistic effect between strong acidity and a suitable pore diameter of the silica catalyst may be responsible for its high activity. In addition, the catalyst was recyclable and showed excellent stability during the recycle catalytic runs.