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Adaptable Reactors for Resource- and Energy-Efficient Methane Valorisation

Periodic Reporting for period 3 - ADREM (Adaptable Reactors for Resource- and Energy-Efficient Methane Valorisation)

Reporting period: 2018-10-01 to 2019-09-30

The societal importance of methane as the source of energy and chemicals in the coming decennia cannot be overestimated. The enormous reserves, its potential contribution to improved environmental sustainability, and lower overall costs point to natural gas as the dominating primary source for energy and chemicals in the near future. Small natural gas reservoirs, shale gas, coalbed methane, agricultural biogas and deep-sea methane hydrates contribute to the great diversity of methane sources. This diversity creates a need to develop modular, flexible catalytic reactor systems capable of valorizing methane to longer hydrocarbons and of operating with changing methane feedstocks in various environments.

The main goal of ADREM was the development of a highly innovative, economically attractive and resource- and energy-efficient valorisation process of variable methane feedstocks to higher hydrocarbons and liquid fuels. The project focused on the development of new and intensified adaptable catalytic reactor systems for flexible and decentralized production at high process performance. The ADREM consortium developed highly innovative, economically attractive and environmentally friendly process and equipment concepts for efficient transformation of methane into valuable chemicals and liquid fuels to be run in the long term on green electricity.

As the main conclusion from the project, our research effort has proven the applicability of several novel, electricity-based reactor concepts to the valorisation of methane. We have successfully tested the selected reactors under the industrially relevant conditions and have identified the elements that need to be addressed in the follow-up research in order to bring the developed concepts to commercialization. The new reactor concepts will enable beneficial utilization of methane from diverse, distributed, small- to-medium-scale sources that could not be utilized until now in an economically feasible way. Among other things, the ADREM reactors will provide means for conversion of methane in cases when it presently has to be flared or released because of lacking connections to gas pipelines. This presents a strong positive environmental impact, which could be still increased when using renewable electricity as a source for operation of the ADREM reactors.
Within the project duration the ADREM project focused on the development, construction and testing of 4 reactor technology concepts (WP1-4) and the associated catalysts (WP5):

• WP1: Two microwave-heating systems were designed to convert methane via non-oxidative coupling mechanism, i.e. Travelling Wave Reactor (TWR) at TU Delft and Multi-stage Monomodal microwave reactor (MMR) at University of Zaragoza.
• WP2: Two nanosecond plasma reactors enabling in situ plasma-catalyst integration and plasma-followed-by catalyst configuration have been constructed at KU Leuven.
• WP3: A gas-solid vortex reactor in a static geometry, a novel reactor technology, for performing oxidative coupling of methane (OCM) was designed and developed at Ghent University.
• WP4: Two plasma reactors, including spark plasma reactor were developed at National Institute of Chemistry.

After three years of initial research, two of the above reactor concepts, the multi-stage monomodal microwave reactor and the nano-second plasma reactor, have been selected for the Technology Readiness Level 5 testing under industrially relevant conditions. The tests included a continuous long-term reactor operation and were the first such tests ever carried out in those types of reactors. Both test programs concerned the non-oxidative coupling of methane and were successfully executed. The microwave reactor was shown to run without human intervention for 295 hours and to produce benzene in amounts close to expected values from the lab experiments. The plasma reactor has proven its capability for non-oxidative methane coupling into C2 products under industrially relevant condition over >200 hours of automated operation. The continuing research on the remaining reactor concepts that were not selected to the TRL5 testing, has shown their potential applicability in other methane valorisation chemistries.

The research results of the project were disseminated in numerous scientific papers and conference presentations, including International Symposium on Chemical Reaction Engineering (ISCRE25, Florence 2018), the European Congress of Chemical Engineering (ECCE, Florence 2019) and the International Conference on Unconventional Catalysis, Reactors and Applications (UCRA, Zaragoza 2019)
ADREM addresses current and future important societal challenges. Novel reactor systems developed in the project will provide indeed novel means for the conversion of methane in cases when it presently has to be flared or released because of lacking or non-economic connections to gas pipelines. This presents a strong positive environmental impact, which will be increased even further when using renewable electricity as a source for operation of the new reactors.

ADREM aims at achieving a threefold impact in technologically, economically and environmentally important sectors:
• Monetary savings of more than 10% compared to conventional processes are expected In addition, technology developed within the ADREM program will facilitate the exploitation of unconventional methane sources not profitable nowadays.
• Processing technologies based on recent research on Process Intensification applying flexible modular one-step process with high selectivity for treatment of methane from various sources.
• Modular (and also containerized and mobile) reactors permitting flexible adaptation of the plant size to demand and also utilizing smaller or temporary sources of methane or other feeds. This will expand the range of processible sources beyond present market limits.

ADREM aims at achieving an impact through
• on-site valorisation of methane from diverse sources,
• filling the processing gap of methane to avoid flaring,
• decreased carbon footprint, and
• increased resource and energy efficiency
leading to several savings:
• 20% less emissions
• 20% less energy intensity
• 10% better overall resource efficiency

ADREM will contribute to a substantial increase in the competitiveness of European industry by:
• Providing to the engineering companies a new generation of processing tools
• Offering to the end-users new cost effective processes
• Opening the possibilities for using the new PI-technologies and components for other innovative applications

The innovative modular PI concepts will enable utilization of smaller sources of methane, contributing to decentralized creation of employment. If ADREM is successful in developing compact processes to treat coal gas and bio-methane, then areas in decline like former and current coal mining areas and some rural areas would profit of it, since not only the energetic utilization of these resources but also the production of feed for chemical industry could contribute to valorisation of these resources. A strong contribution to the mitigation of environmental loads would arise from applications in offshore oil and gas production e.g. by diminishing the amounts of flared gas.
ADREM reactor technologies