In the context of a carbon neutral economy, catalytic CO hydrogenation to methanol is one crucial technology for CO mitigation providing solutions for manufacturing future fuels, chemicals, and materials. However, most of the presently known catalyst systems are used at temperatures over 220 °C, which limits the theoretical yield of methanol production due to the exothermic nature of this transformation. In this review, we summarize state-of-the-art catalysts, focusing on the rationales behind, for CO hydrogenation to methanol at temperatures lower than 170 °C. Both hydrogenation with homogeneous and heterogeneous catalysts is covered. Typically, additives (alcohols, amines or aminoalcohols) are used to transform CO into intermediates, which can further be reduced into methanol. In the first part, molecular catalysts are discussed, organized into: (1) monofunctional, (2) M/NH bifunctional, and (3) aromatization-dearomatization bifunctional molecular catalysts. In the second part, heterogeneous catalysts are elaborated, organized into: (1) metal/metal or metal/support, (2) active-site/N or active-site/OH bifunctional heterogeneous catalysts, and (3) cooperation of catalysts and additives in a tandem process via crucial intermediates. Although many insights have been gained in this transformation, in particular for molecular catalysts, the mechanisms in the presence of heterogeneous catalysts remain descriptive and insights unclear.
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http://dx.doi.org/10.1039/d0cs01331e | DOI Listing |
Nat Commun
January 2025
Wuhan National Laboratory for Optoelectronics, School of Optoelectronic Science and Engineering, Huazhong University of Science and Technology, Wuhan, PR China.
Active and stable electrocatalysts are essential for hydrogen production from alkaline water electrolysis. However, precisely controlling the interaction between electrocatalysts and reaction intermediates (HO*, H*, and *OH) remains challenging. Here, we demonstrate an yttrium-doped NiMo-MoO heterogenous electrocatalyst that efficiently promotes water dissociation and accelerates the intermediate adsorption/desorption dynamics in alkaline electrolytes.
View Article and Find Full Text PDFEnviron Sci Technol
January 2025
State Key Laboratory of Heavy Oil Processing, Key Laboratory of Optical Detection Technology for Oil and Gas, College of Science, China University of Petroleum, Beijing 102249, PR China.
The purification efficiency of autoexhaust carbon strongly depends on the heterogeneous interface structure between active metal and oxide, which can modulate the local electronic structure of defect sites to promote the activation of reactant molecules. Herein, the high-dispersion CuO clusters supported on the well-defined CeO nanorods were prepared using the complex deposition slow method. The formation of heteroatomic Cu-O-Ce interfacial structural units as active sites can capture electrons to achieve activation of the NO and O molecules.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
The Institute for Advanced Studies, Wuhan University, Wuhan, Hubei 430072, People's Republic of China.
Deuterated compounds have broad applications across various fields, with dehalogenative deuteration serving as an efficient method to obtain these molecules. However, the diverse electronic structures of active sites in the heterogeneous system and the limited recyclability in the homogeneous system significantly hinder the advancement of dehalogenative deuteration. In this study, we present a catalyst composed of copper single-atom sites anchored within an ordered mesoporous nitrogen-doped carbon matrix, synthesized via a mesopore confinement method.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
East China University of Science and Technology, Key Laboratory for Advanced Materials and Institute of Fine Chemicals, 130 Meilong Road, 200237, Shanghai, CHINA.
Nanoconfinement at the interface of heterogeneous Fenton-like catalysts offers promising avenues for advancing oxidation processes in water purification. Herein, we introduce a template-free strategy for synthesizing nanoconfined catalysts from municipal sludge (S-NCCs), specifically engineered to optimize reactive oxygen species (ROS) generation and utilization for rapid pollutant degradation. Using selective hydrofluoric acid corrosion, we create an architecture that confines atomically dispersed Fe centers within a micro-mesoporous carbon matrix in situ.
View Article and Find Full Text PDFChempluschem
January 2025
L V Pisarzhevskii Institute of Physical Chemistry NAS of Ukraine: Institut fiziceskoj himii imeni L V Pisarzevskogo Nacional'na akademia nauk Ukraini, Department of free radicals, UKRAINE.
This study unveils a novel property of polyaniline by establishing its catalytic activity in heterogeneous hydrogenation with molecular hydrogen. Polyaniline was activated by heat-treating at different temperatures in a hydrogen atmosphere. The sample treated at 300 °C exhibited the highest catalytic activity for ethylene hydrogenation in the gas phase at atmospheric pressure and for p-nitrotoluene or α-methylstyrene hydrogenation in the liquid phase.
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