The water-gas shift (WGS) reaction (where carbon monoxide plus water yields dihydrogen and carbon dioxide) is an essential process for hydrogen generation and carbon monoxide removal in various energy-related chemical operations. This equilibrium-limited reaction is favored at a low working temperature. Potential application in fuel cells also requires a WGS catalyst to be highly active, stable, and energy-efficient and to match the working temperature of on-site hydrogen generation and consumption units. We synthesized layered gold (Au) clusters on a molybdenum carbide (α-MoC) substrate to create an interfacial catalyst system for the ultralow-temperature WGS reaction. Water was activated over α-MoC at 303 kelvin, whereas carbon monoxide adsorbed on adjacent Au sites was apt to react with surface hydroxyl groups formed from water splitting, leading to a high WGS activity at low temperatures.
Supercapacitors attract great interest because of the increasing and urgent demand for environment‐friendly high‐power energy sources. Ti3C2, a member of MXene family, is a promising electrode material for supercapacitors owing to its excellent chemical and physical properties. However, the highest gravimetric capacitance of the MXene‐based electrodes is still relatively low (245 F g−1) and the key challenge to improve this is to exploit more pseudocapacitance by increasing the active site concentration. Here, a method to significantly improve the gravimetric capacitance of Ti3C2Tx MXenes by cation intercalation and surface modification is reported. After K+ intercalation and terminal groups (OH−/F−) removing , the intercalation pseudocapacitance is three times higher than the pristine MXene, and MXene sheets exhibit a significant enhancement (about 211% of the origin) in the gravimetric capacitance (517 F g−1 at a discharge rate of 1 A g−1). Moreover, the as‐prepared electrodes show above 99% retention over 10 000 cycles. This improved electrochemical performance is attributed to the large interlayer voids of Ti3C2 and lowest terminated surface group concentration. This study demonstrates a new strategy applicable to other MXenes (Ti2CTx, Nb2CTx, etc.) in maximizing their potential applications in energy storage.
A one-step ligand-free method based on an adsorption-precipitation process was developed to fabricate iridium/cerium oxide (Ir/CeO ) nanocatalysts. Ir species demonstrated a strong metal-support interaction (SMSI) with the CeO substrate. The chemical state of Ir could be finely tuned by altering the loading of the metal. In the carbon dioxide (CO ) hydrogenation reaction it was shown that the chemical state of Ir species-induced by a SMSI-has a major impact on the reaction selectivity. Direct evidence is provided indicating that a single-site catalyst is not a prerequisite for inhibition of methanation and sole production of carbon monoxide (CO) in CO hydrogenation. Instead, modulation of the chemical state of metal species by a strong metal-support interaction is more important for regulation of the observed selectivity (metallic Ir particles select for methane while partially oxidized Ir species select for CO production). The study provides insight into heterogeneous catalysts at nano, sub-nano, and atomic scales.
Zn- and Na-modulated Fe catalysts were fabricated by a simple coprecipitation/washing method. Zn greatly changed the size of iron species, serving as the structural promoter, while the existence of Na on the surface of the Fe catalyst alters the electronic structure, making the catalyst very active for CO activation. Most importantly, the electronic structure of the catalyst surface suppresses the hydrogenation of double bonds and promotes desorption of products, which renders the catalyst unexpectedly reactive toward alkenes-especially C5+ alkenes (with more than 50% selectivity in hydrocarbons)-while lowering the selectivity for undesired products. This study enriches C1 chemistry and the design of highly selective new catalysts for high-value chemicals.
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