Although considerable progress has been made in carbon dioxide (CO) hydrogenation to various C chemicals, it is still a great challenge to synthesize value-added products with two or more carbons, such as gasoline, directly from CO because of the extreme inertness of CO and a high C-C coupling barrier. Here we present a bifunctional catalyst composed of reducible indium oxides (InO) and zeolites that yields a high selectivity to gasoline-range hydrocarbons (78.6%) with a very low methane selectivity (1%). The oxygen vacancies on the InO surfaces activate CO and hydrogen to form methanol, and C-C coupling subsequently occurs inside zeolite pores to produce gasoline-range hydrocarbons with a high octane number. The proximity of these two components plays a crucial role in suppressing the undesired reverse water gas shift reaction and giving a high selectivity for gasoline-range hydrocarbons. Moreover, the pellet catalyst exhibits a much better performance during an industry-relevant test, which suggests promising prospects for industrial applications.

Direct conversion of carbon dioxide (CO2) into lower olefins (C2 =–C4 =), generally referring to ethylene, propylene, and butylene, is highly attractive as a sustainable production route for its great significance in greenhouse gas control and fossil fuel substitution, but such a route always tends to be low in selectivity toward olefins. Here we present a bifunctional catalysis process that offers C2 =–C4 = selectivity as high as 80% and C2–C4 selectivity around 93% at more than 35% CO2 conversion. This is achieved by a bifunctional catalyst composed of indium–zirconium composite oxide and SAPO-34 zeolite, which is responsible for CO2 activation and selective C–C coupling, respectively. We demonstrate that both the precise control of oxygen vacancies on the oxide surface and the integration manner of the components are crucial in the direct production of lower olefins from CO2 hydrogenation. No obvious deactivation is observed over 150 h, indicating a promising potential for industrial application.

As important industrial materials, microporous zeolites are necessarily synthesized in the presence of solvents such as in hydrothermal, solvothermal, and ionothermal routes. We demonstrate here a simple and generalized solvent-free route for synthesizing various types of zeolites by mixing, grinding, and heating solid raw materials. Compared with conventional hydrothermal route, the avoidance of solvents in the synthesis not only significantly reduces the waste production, but also greatly increases the yield of zeolite products. In addition, the use of starting solid raw materials remarkably enhances the synthesis efficiency and reduces the use of raw materials, energy, and costs.

Low-cost copper-amine complex was rationally designed to be a novel template for one-pot synthesis of Cu-SSZ-13 zeolites. Proper confirmation and appropriate size make this complex fit well with CHA cages as an efficient template. The products exhibit superior catalytic performance on NH(3)-SCR reaction.

Mesoporous zeolites are useful solid catalysts for conversion of bulky molecules because they offer fast mass transfer along with size and shape selectivity. We report here the successful synthesis of mesoporous aluminosilicate zeolite Beta from a commercial cationic polymer that acts as a dual-function template to generate zeolitic micropores and mesopores simultaneously. This is the first demonstration of a single nonsurfactant polymer acting as such a template. Using high-resolution electron microscopy and tomography, we discovered that the resulting material (Beta-MS) has abundant and highly interconnected mesopores. More importantly, we demonstrated using a three-dimensional electron diffraction technique that each Beta-MS particle is a single crystal, whereas most previously reported mesoporous zeolites are comprised of nanosized zeolitic grains with random orientations. The use of nonsurfactant templates is essential to gaining single-crystalline mesoporous zeolites. The single-crystalline nature endows Beta-MS with better hydrothermal stability compared with surfactant-derived mesoporous zeolite Beta. Beta-MS also exhibited remarkably higher catalytic activity than did conventional zeolite Beta in acid-catalyzed reactions involving large molecules.

We demonstrate here a seed-directed synthesis (SDS) of Beta, Levyne, and Heulandite zeolites in the absence of organotemplates, where the seeds drive crystallization of the zeolites. Compared with conventional Beta synthesized in the presence of organic templates, Beta-SDS exhibits large textural parameters, stable Al species, and unprecedentedly high density of active sites, resulting in superior catalytic activity and selectivity for valuable products in catalysis.

Microporous crystalline aluminosilicate and silicoaluminophosphate zeolites are currently regarded as the most useful zeolite catalysts for industrial processes. [1] For example, aluminosilicate Y zeolite is efficient for fluid catalytic cracking, [2] and silicoaluminophosphate SAPO-34 zeolite is a selective catalyst for the formation of light olefins from methanol. [3] Notably, the synthesis of these zeolites usually requires the presence of solvents such as water and alcohols under hydrothermal, solvothermal, or ionothermal conditions. [1][2][3][4][5][6][7][8][9][10][11][12] The use of solvents normally results in polluted water, reduced synthesis efficiency owing to autoclave space being used by the solvent, and generates high pressure under hightemperature solvothermal conditions. [4] The ionothermal route, which has been successfully developed for synthesizing aluminophosphate-based zeolites, can effectively eliminate the high pressure problem, because of the low vapor pressure of ionic liquids. [5,6] Recently, Ren et al. reported the solventfree synthesis of aluminosilicate zeolites with the advantage of reducing waste production and increasing zeolite yield, as well as eliminating high pressure. [4b] Morris et al. have also highlighted the importance of solventless synthesis, [7] but this route has still not been successfully applied to the synthesis of aluminophosphate-based zeolites.Herein, we report the solvent-free synthesis of silicoaluminophosphate (SAPO-34, SAPO-11, SAPO-20, and SAPO-43), aluminophosphate (APO-11), and heteroatom-containing aluminophosphate (M-APO-11 and M-SAPO-46; M = Co or Mg) zeolites by mixing, grinding, and heating the raw materials. The solvent-free synthesis of SAPO-34 (S-SAPO-34) is carefully investigated as a model reaction. Importantly, S-SAPO-34 exhibits good catalytic performance in catalytic tests for methanol-to-olefin (MTO) conversion. Figure 1 shows X-ray diffraction (XRD) pattern, N 2 sorption isotherms, scanning electron microscopy (SEM), and transmission electron microscopy (TEM) images of calcined S-SAPO-34. XRD patterns show well-resolved peaks in the range of 4-408 (Figure 1 A), which are in good agreement with that of a CHA zeolite structure. [8] N 2 sorption isotherms of the sample (Figure 1 B) exhibit a steep increase in the curve at a relative pressure of 10 À6 < P/P 0 < 0.01, which is due to the filling of micropores. [4a] Additionally, at a relative pressure of 0.50-0.98, a hysteresis loop can be observed, which suggests that the sample is both meso-and macroporous. [9] Accordingly, the sample Barrett-Joyner-Halenda (BJH) pore-size distribution appears at 11 nm and ca. 100 nm (Figure 1 C). The Brunauer-Emmett-Teller (BET) surface area and pore volume are 459 m 2 g À1 and 0.27 cm 3 g À1 , respectively. Figure 1 D and E show low and high magnification SEM images of the sample. The low magnification image (Figure 1 D) shows that the sample has very uniform cubic morphology, with particle sizes of 10-30 mm. The high magnification image (Figure 1 E) clea...

Xiao and colleagues successfully designed a powerful siliceous zeolite support and a core-shell structure, which is achieved by fixing RhMn nanoparticles within Silicate-1 zeolite crystals (RhMn@S-1), could remarkably boost the ethanol production from direct syngas conversion. C 2 -oxygenate selectivity of 88.3% in the total oxygenates was obtained at 42.4% CO conversion, decidedly outperforming the previous Rh-based catalysts. This work provides a new route for design and preparation of highly efficient catalyst for ethanol production from syngas.