A series of layered Co-Al-O catalysts derived from hydrotalcites for low-temperature CO2 methanation were prepared via a hydrothermal method and reduced at 500, 550, 600, 650, and 700 °C, respectively. The characterisation results from XPS and CO2-TPD revealed that the Co0 content and basic sites over these catalysts were firstly increased and then decreased with the reduction temperature increasing, which led to the efficient dissociation of H2 and CO2 adsorption. In situ DRIFTS measurements revealed that the formation of CH4 proceeded via the hydrogenation of carbonate and formate as intermediates. A superior catalytic performance of Co-Al-O-600 catalyst for CO2 methanation was achieved with a CO2 conversion of 74% and a CH4 selectivity of 99% at low temperature of 250 °C. Moreover, it exhibited excellent resistance to coking and sintering upon a 240 h time on stream operation. 

Highly stable and selective layered Co-Al-O catalysts for low-temperature CO2 methanation

Ruthenium (Ru) is the one of the most promising catalysts for polyolefin hydrogenolysis. Its performance varies widely with the support, but the reasons remain unknown. Here, we introduce a simple synthetic strategy (using ammonia as a modulator) to tune metal-support interactions and apply it to Ru deposited on titania (TiO2). We demonstrate that combining deuterium nuclear magnetic resonance spectroscopy with temperature variation and density functional theory can reveal the complex nature, binding strength, and H amount. H2 activation occurs heterolytically, leading to a hydride on Ru, an H+ on the nearest oxygen, and a partially positively charged Ru. This leads to partial reduction of TiO2 and high coverages of H for spillover, showcasing a threefold increase in hydrogenolysis rates. This result points to the key role of the surface hydrogen coverage in improving hydrogenolysis catalyst performance. 

/pdf/electronic-modulation-of-metal-support-interactions-improves-3telthdy.pdf

Electronic modulation of metal-support interactions improves polypropylene hydrogenolysis over ruthenium catalysts

Plasmon-Enhanced Photocatalytic Properties of Au/ZnO Nanowires

Research interest in single-atom catalysts (SACs) has been continuously increasing. However, the lack of understanding of the dynamic behaviors of SACs during applications hinders catalyst development and mechanistic understanding. Herein, we report on the evolution of active sites over Pd/TiO2-anatase SAC (Pd1/TiO2) in the reverse water-gas shift (rWGS) reaction. Combining kinetics, in situ characterization, and theory, we show that at T ≥ 350 °C, the reduction of TiO2 by H2 alters the coordination environment of Pd, creating Pd sites with partially cleaved Pd-O interfacial bonds and a unique electronic structure that exhibit high intrinsic rWGS activity through the carboxyl pathway. The activation by H2 is accompanied by the partial sintering of single Pd atoms (Pd1) into disordered, flat, ∼1 nm diameter clusters (Pdn). The highly active Pd sites in the new coordination environment under H2 are eliminated by oxidation, which, when performed at a high temperature, also redisperses Pdn and facilitates the reduction of TiO2. In contrast, Pd1 sinters into crystalline, ∼5 nm particles (PdNP) during CO treatment, deactivating Pd1/TiO2. During the rWGS reaction, the two Pd evolution pathways coexist. The activation by H2 dominates, leading to the increasing rate with time-on-stream, and steady-state Pd active sites similar to the ones formed under H2. This work demonstrates how the coordination environment and nuclearity of metal sites on a SAC evolve during catalysis and pretreatments and how their activity is modulated by these behaviors. These insights on SAC dynamics and the structure-function relationship are valuable to mechanistic understanding and catalyst design.

Dynamic Evolution of Palladium Single Atoms on Anatase Titania Support Determines the Reverse Water-Gas Shift Activity.

Suppressing byproduct formation for high selective CO2 reduction over optimized Ni/TiO2 based catalysts

Methanol synthesis by CO2 reduction is an important approach for energy storage. Aiming at a reduction of the catalyst mass in technical applications, we have investigated the influence of increasing Au loading on the performance of Au/ZnO in methanol and CO formation from CO2 reduction. Using the same type of ZnO support, increased Au loading resulted also in a pronounced increase in Au particle size. The Au-mass-normalized reaction rate for methanol formation and TOF decrease with increasing Au loading/particle size, while the selectivity for methanol formation increases. CO adsorption monitored by in situ FTIR revealed a pronounced decrease of the accessible Au surface area during reaction, independent of the Au loading, pointing to a partial encapsulation of the Au nanoparticles by a partly reduced ZnOx, as described by SMSI effects. Possible reasons responsible for these effects and Au loading/size effects therein are discussed, strategies for future work are outlined.

Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size

Steering the selectivity in CO2 reduction on highly active Ru/TiO2 catalysts: Support particle size effects

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Performance of Au/ZnO catalysts in CO2 reduction to methanol: Varying the Au loading / Au particle size

Steering the selectivity in CO2 reduction on highly active Ru/TiO2 catalysts: Support particle size effects