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This study presents a comprehensive, multidisciplinary approach to high-throughput screening (HTS) of metal–organic frameworks (MOFs) for efficient ammonia-based green hydrogen production. Previous HTS methods, relying on molecular simulations, often estimate adsorption uptakes under constant conditions, leading to inadequate evaluation of MOFs for practical applications where competitive adsorption and varying operating conditions are critical. To address this limitation, we propose a multidisciplinary HTS method employing an efficient computational algorithm that minimizes the number of molecular simulations while generating isotherm models across a wide pressure range. Our algorithm strategically selects simulations for further analysis based on initial results. Using this innovative approach, we screened 12,020 MOFs. Furthermore, as the next step of the multidisciplinary approach, we performed pressure swing adsorption (PSA) process simulations to assess MOFs' potential for purifying green hydrogen derived from decomposed ammonia, which can be produced by sustainable energy sources and transported intercontinentally. The top-performing MOFs were evaluated for stability based on literature data and MOFSimplify, a neural network model estimating thermal stability. By considering adsorption process operation and MOF stability, the proposed HTS methodology identified 10 high-performing materials, with RAVXIX ranking as the top adsorbent. This comprehensive evaluation advances the search for efficient MOFs in green hydrogen production, contributing to the development of a more sustainable hydrogen-based economy. • A multidisciplinary high-throughput screening method using an novel algorithm was proposed. • The proposed HTS considers molecular and process simulations and structural stability. • This study presents MOFs best suited for green NH 3 -based H 2 separation. • Best-performing MOFs based on PSA simulation and stability were found for green NH 3 -based H 2 separation. [ABSTRACT FROM AUTHOR]

Because green ammonia is an emerging transportation medium for carbon-free hydrogen, technologies for efficient and cost-effective separation and purification of green hydrogen have attracted significant attention in recent years. Among the various options for hydrogen separation, pressure swing adsorption (PSA) has the highest technology readiness level, but the optimal adsorbent for this application is still under investigation. This study evaluates the viability of covalent organic framework (COF) adsorbents for ammonia-based green hydrogen separation processes. The feasibility of the adsorbents was estimated based on the economic analysis of the entire green hydrogen production process with a newly proposed multiscale high-throughput screening (HTS) approach. This approach addresses an existing knowledge gap, where the molecular- and process-scale viewpoints are not fully considered together during adsorbent evaluation. The proposed HTS approach incorporates a new algorithm for simulations with reduced computational cost and a procedure for estimating the economic viability of the adsorbents. The results show that among 648 COFs in a COF database, MPCOF was the most efficient for ammonia-based green H 2 separation with a H 2 recovery of 72% and levelized cost of USD 8.30/kg H 2. This result was obtained with only 31% of the computational cost required by an existing HTS approach. • Novel high-throughput screening (HTS) method is proposed based on multiscale simulation. • The proposed HTS spans from molecular- to process- scale including economic analysis. • Optimal adsorbent for H 2 production from green NH 3 is identified with the proposed HTS. • New isotherm fitting algorithm in HTS offers higher accuracy and computational efficiency. [ABSTRACT FROM AUTHOR]

[Display omitted] • An induction heating-based reactor for ammonia decomposition is developed. • The reactor produced an ammonia conversion of >90.0 % at 600 °C and 7 bar. • Proposed process achieves a 150 Nm3/h carbon-free green hydrogen production. • Exergy analysis indicated an exergy efficiency of 54.21% for the overall process. • The levelized cost of hydrogen (LCOH) was calculated to be 6.98 USD/kgH 2. This study presents an induction heating-based reactor for ammonia decomposition and to achieve a 150 Nm3/h carbon-free green hydrogen production process. The developed metallic monolith reactor acts by increasing the reactor temperature through an electromagnetic induction method using renewable-based electricity. As a result, hydrogen is produced without the generation of air pollutants such as CO 2 , which are formed via the conventional production pathway. Furthermore, techno-economic analysis was conducted based on exergy and economic analysis to evaluate the feasibility of the developed process. Experimentally, the proposed reactor showed an ammonia conversion of 90.0 % at 600 ℃ and 7 barg. Exergy analysis indicated that the total unused exergy accounted for 45.79 % of the total exergy input, giving an exergy efficiency of 54.21 % for the overall process. Furthermore, the CAPEX and OPEX values are calculated as 1,599,567 USD and 644,719 USD/y, respectively; therefore, the levelized cost of hydrogen (LCOH) was calculated to be 6.98 USD/kgH 2. This study also demonstrated that the LCOH varies with the ammonia feed price and the process capacity, and so it would be expected to decrease from 6.98 to 5.33 USD/kgH 2 as the hydrogen production capacity is increased from 150 to 500 Nm3/h. Overall, our results confirm the feasibility of carbon-free green hydrogen production on on-site hydrogen refueling stations, and they will be expected to advance the development of an environmental hydrogen economy. [ABSTRACT FROM AUTHOR]