Sulfur-based metal-organic frameworks (MOFs) and coordination polymers (CPs) are an emerging class of hybrid materials that have received growing attention due to their magnetic, conductive, and catalytic properties with potential applications in electrocatalysis and energy storage. In this work, we report a high-throughput virtual screening protocol to predict the synthesizability of candidate metal-sulfur MOFs/CPs by computing the thermodynamically stable structures resulting from a particular combination of metal cluster, linker, cation, and synthetic conditions. Free energies are computed by using all-atom classical mechanical thermodynamic integration. Low-free-energy structures are refined using ab initio density functional theory, and pair distribution functions and powder X-ray diffraction patterns are calculated to complement and guide experimental structure determination. We validate the computational approach by retrospective predictions of the stable structure produced by experimental syntheses, and a subsequent screen predicts Fe4S4-BDT-TPP as a new thermodynamically stable one-dimensional (1D) CP comprising a redox-active Fe4S4 cluster, a 1,4-benzenedithiolate (BDT) linker, and a tetraphenylphosphonium (TPP) countercation. This material is experimentally synthesized, and the 1D chain structure of the crystal is confirmed using microcrystal electron diffraction. The computational screening pipeline is generically transferable to neutral and ionic MOFs/CPs comprising arbitrary metal clusters, linkers, cations, and synthetic conditions, and we make it freely available as an open source tool to guide and accelerate the discovery and engineering of novel porous materials.
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Theoret & Computat Biophys Grp, NIH Resource Macromol Modeling & Visualizat, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA
Univ Illinois, Ctr Biophys & Quantitat Biol, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Park, Hyun
;
Yan, Xiaoli
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机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Multiscale Mat & Mfg Lab, Chicago, IL 60607 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Yan, Xiaoli
;
Zhu, Ruijie
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Zhu, Ruijie
;
Huerta, Eliu A.
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Chicago, Dept Comp Sci, Chicago, IL 60637 USA
Univ Illinois, Dept Phys, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Huerta, Eliu A.
;
Chaudhuri, Santanu
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Multiscale Mat & Mfg Lab, Chicago, IL 60607 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Chaudhuri, Santanu
;
Cooper, Donny
论文数: 0引用数: 0
h-index: 0
机构:
TotalEnergies EP Res & Technol USA LLC, Data Sci & AI Dept, Computat Sci & Engn, Houston, TX 77002 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Cooper, Donny
;
Foster, Ian
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Chicago, Dept Comp Sci, Chicago, IL 60637 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Foster, Ian
;
Tajkhorshid, Emad
论文数: 0引用数: 0
h-index: 0
机构:
Univ Illinois, Theoret & Computat Biophys Grp, NIH Resource Macromol Modeling & Visualizat, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA
Univ Illinois, Ctr Biophys & Quantitat Biol, Urbana, IL 61801 USA
Univ Illinois, Dept Biochem, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Univ Zurich, Dept Chem, CH-8057 Zurich, SwitzerlandStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Pascanu, Vlad
;
Miera, Greco Gonzalez
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Nagoya Univ, Inst Transformat Biomol WPI ITbM, Chikusa Ku, Nagoya, Aichi 4648602, Japan
Nagoya Univ, Grad Sch Sci, Chikusa Ku, Nagoya, Aichi 4648602, JapanStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Miera, Greco Gonzalez
;
Inge, A. Ken
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Mat & Environm Chem, SE-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Inge, A. Ken
;
Martin-Matute, Belen
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
机构:
CSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Leibniz Inst Katalyse e V, Albert Einstein Str 29a, D-18059 Rostock, GermanyCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Peng, Yong
;
Sanati, Soheila
论文数: 0引用数: 0
h-index: 0
机构:
Tarbiat Modares Univ, Fac Basic Sci, Dept Chem, Tehran 14115175, IranCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Sanati, Soheila
;
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Morsali, Ali
;
Garcia, Hermenegildo
论文数: 0引用数: 0
h-index: 0
机构:
CSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, SpainCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Theoret & Computat Biophys Grp, NIH Resource Macromol Modeling & Visualizat, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA
Univ Illinois, Ctr Biophys & Quantitat Biol, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Park, Hyun
;
Yan, Xiaoli
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Multiscale Mat & Mfg Lab, Chicago, IL 60607 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Yan, Xiaoli
;
Zhu, Ruijie
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Zhu, Ruijie
;
Huerta, Eliu A.
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Chicago, Dept Comp Sci, Chicago, IL 60637 USA
Univ Illinois, Dept Phys, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Huerta, Eliu A.
;
Chaudhuri, Santanu
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Illinois, Multiscale Mat & Mfg Lab, Chicago, IL 60607 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Chaudhuri, Santanu
;
Cooper, Donny
论文数: 0引用数: 0
h-index: 0
机构:
TotalEnergies EP Res & Technol USA LLC, Data Sci & AI Dept, Computat Sci & Engn, Houston, TX 77002 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Cooper, Donny
;
Foster, Ian
论文数: 0引用数: 0
h-index: 0
机构:
Argonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Univ Chicago, Dept Comp Sci, Chicago, IL 60637 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
Foster, Ian
;
Tajkhorshid, Emad
论文数: 0引用数: 0
h-index: 0
机构:
Univ Illinois, Theoret & Computat Biophys Grp, NIH Resource Macromol Modeling & Visualizat, Beckman Inst Adv Sci & Technol, Urbana, IL 61801 USA
Univ Illinois, Ctr Biophys & Quantitat Biol, Urbana, IL 61801 USA
Univ Illinois, Dept Biochem, Urbana, IL 61801 USAArgonne Natl Lab, Data Sci & Learning Div, Lemont, IL 60439 USA
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Univ Zurich, Dept Chem, CH-8057 Zurich, SwitzerlandStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Pascanu, Vlad
;
Miera, Greco Gonzalez
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Nagoya Univ, Inst Transformat Biomol WPI ITbM, Chikusa Ku, Nagoya, Aichi 4648602, Japan
Nagoya Univ, Grad Sch Sci, Chikusa Ku, Nagoya, Aichi 4648602, JapanStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Miera, Greco Gonzalez
;
Inge, A. Ken
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Mat & Environm Chem, SE-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
Inge, A. Ken
;
Martin-Matute, Belen
论文数: 0引用数: 0
h-index: 0
机构:
Stockholm Univ, Dept Organ Chem, SE-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, SE-10691 Stockholm, Sweden
机构:
CSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Leibniz Inst Katalyse e V, Albert Einstein Str 29a, D-18059 Rostock, GermanyCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Peng, Yong
;
Sanati, Soheila
论文数: 0引用数: 0
h-index: 0
机构:
Tarbiat Modares Univ, Fac Basic Sci, Dept Chem, Tehran 14115175, IranCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain
Sanati, Soheila
;
论文数: 引用数:
h-index:
机构:
Morsali, Ali
;
Garcia, Hermenegildo
论文数: 0引用数: 0
h-index: 0
机构:
CSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, SpainCSIV UPV, Inst Tecnol Quim, Av Delos Naranjos S N, Valencia 46022, Spain