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Although ethylene (C2H4) is one of the most critical chemicals used as a feedstock in artificial plastic chemistry fields, it is challenging to obtain high‐purity C2H4 gas without any trace ethane (C2H6) by the oil cracking process. Adsorptive separation using C2H6‐selective adsorbents is beneficial because it directly produces high‐purity C2H4 in a single step. Herein, Ni(IN)2 (HIN = isonicotinic acid) is computationally discovered as a promising adsorbent with the assistance of the multiscale high‐throughput computational screening workflow and Computation‐Ready, Experimental (CoRE) metal–organic framework (MOF) 2019 database. Ni(IN)2 is subsequently synthesized and tested to show the ideal adsorbed solution theory (IAST) selectivity of 2.45 at 1 bar for a C2H6/C2H4 mixture (1:15), which is one of the top‐performing selectivity values reported for C2H6‐selective MOFs as well as excellent recyclability, suggesting that this material is a promising C2H6‐selective adsorbent. Process‐level simulation results based on experimental isotherms demonstrate that the material is one of the top materials reported to date for ethane/ethylene separation under the conditions considered in this work. [ABSTRACT FROM AUTHOR]

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]

In this work, we proposed multi-scale screening, which employs both molecular and process-level methods, to identify high-performing MOFs for energy-efficient separation of S F 6 and N 2 mixture. Grand canonical Monte Carlo (GCMC) simulations were combined with ideal adsorption process simulation to computationally screen 2890 metal–organic frameworks (MOFs) for adsorptive separation of S F 6 /N 2. More than 150 high-performing MOFs were identified based on the GCMC simulations at the pressure and vacuum swing conditions, and subsequently evaluated using the ideal adsorption process simulation. 78 out of 86 MOFs selected for the VSA conditions were able to achieve the 90% target purity level of S F 6 , but 62 top-performing MOFs selected for the PSA condition could not reach the purity level with a single train PSA configuration. Cascade PSA configuration was proposed and adopted to improve the purity level. We also investigated the effect of vacuum pump and compressor efficiency on the energy consumption of the process. We found that the top-performing MOFs were able to achieve the 90% purity-level of S F 6 with 0.10–0.4 and 0.5–1.4 MJ per kg of S F 6 for VSA and PSA processes, respectively. Finally, the process-level performance of top-performing MFOs (HKST-1, UiO-67) was evaluated on the basis of the experimental isotherms obtained from the literature, and compared with the other materials reported in the literature (MIL-100(Fe), UiO-66, and zeolite-13X). We found that the results based on the experimental isotherms are in qualitative agreement with the results based on the simulated isotherms. • Multi-scale screening with the molecular- and process-level simulations. • High-throughput GCMC screening of 2890 MOFs for S F 6 /N 2 separation. • 86 and 62 top-performing MOFs were identified under PSA and VSA conditions. • Performance of top MOFs from VSA and PSA compared under different pump efficiency. • Evaluation of top MOFs based on both experimental and simulated isotherms. [ABSTRACT FROM AUTHOR]