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1.
Natl Sci Rev ; 10(9): nwad116, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37565204

RESUMO

The utilization of methane for chemical production, often considered as the future of petrochemistry, historically could not compete economically with conventional processes due to higher investment costs. Achieving sustainability and decarbonization of the downstream industry by integration with a methane-to-chemicals process may provide an opportunity to unlock the future for these technologies. Gas-to-chemicals is an efficient tool to boost the decarbonization potential of renewable energy. While the current implementation of carbon capture utilization and storage (CCUS) technologies is of great importance for industrial decarbonization, a shift to greener CO2-free processes and CO2 utilization from external sources for manufacturing valuable goods is highly preferred. This review outlines potential options for how a methane-to-chemicals process could support decarbonization of the downstream industry.

2.
Angew Chem Int Ed Engl ; 59(44): 19414-19432, 2020 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-32691444

RESUMO

The development of catalysts that can operate under exceptionally harsh and unconventional conditions is of critical importance for the transition of the energy and chemicals industries to low-emission and renewable chemical feedstocks. In this review we will highlight materials and more specifically metal-containing zeolite catalysts that have been tested under harsh reaction conditions such as high temperature light alkane conversion and biomass valorization. Particular attention will be given to studies that explore the stability and recyclability of metal-containing zeolite catalysts operating in continuous modes. Metal-containing zeolites are considered as an important class of catalysts operating outside the comfort zone of current heterogeneous catalytic reactions in both gas and liquid phase reactions. The relationship between the properties of the metal-containing zeolite and catalytic performance will be explored.

3.
Angew Chem Int Ed Engl ; 59(44): 19553-19560, 2020 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-32681561

RESUMO

The current energy transition presents many technological challenges, such as the development of highly stable catalysts. Herein, we report a novel "top-down" synthesis approach for preparation of a single-site Mo-containing nanosized ZSM-5 zeolite which has atomically dispersed framework-molybdenum homogenously distributed through the zeolite crystals. The introduction of Mo heals most of the native point defects in the zeolite structure resulting in an extremely stable material. The important features of this single-site Mo-containing ZSM-5 zeolite are provided by an in-depth spectroscopic and microscopic analysis. The material demonstrates superior thermal (up to 1000 °C), hydrothermal (steaming), and catalytic (converting methane to hydrogen and higher hydrocarbons) stability, maintaining the atomically disperse Mo, structural integrity of the zeolite, and preventing the formation of silanols.

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