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      Does repeat synthesis in materials chemistry obey a power law?

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          Significance

          A key goal of much chemistry and materials research is the creation of new chemicals or materials. Understanding how readily the synthesis of a material can be repeated gives important insight into how a material can be adopted by a technical community or used in practical applications. Surprisingly, little is known about how often the synthesis of new materials gets repeated. In this paper, an extensive analysis of published literature for a specific class of materials, metal-organic frameworks, is used to quantitatively address this issue.

          Abstract

          Finding examples where experimental measurements have been repeated is a powerful strategy for assessing reproducibility of scientific data. Here, we collect quantitative data to assess how often synthesis of a newly reported material is repeated in the scientific literature. We present a simple power-law model for the frequency of repeat syntheses and assess the validity of this model using a specific class of materials, metal-organic frameworks (MOFs). Our data suggest that a power law describes the frequency of repeat synthesis of many MOFs but that a small number of “supermaterials” exist that have been replicated many times more than a power law would predict. Our results also hint that there are many repeat syntheses that have been performed but not reported in the literature, which suggests simple steps that could be taken to greatly increase the number of reports of replicate experiments in materials chemistry.

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          Most cited references27

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          Unusual and highly tunable missing-linker defects in zirconium metal-organic framework UiO-66 and their important effects on gas adsorption.

          UiO-66 is a highly important prototypical zirconium metal-organic framework (MOF) compound because of its excellent stabilities not typically found in common porous MOFs. In its perfect crystal structure, each Zr metal center is fully coordinated by 12 organic linkers to form a highly connected framework. Using high-resolution neutron power diffraction technique, we found the first direct structural evidence showing that real UiO-66 material contains significant amount of missing-linker defects, an unusual phenomenon for MOFs. The concentration of the missing-linker defects is surprisingly high, ∼10% in our sample, effectively reducing the framework connection from 12 to ∼11. We show that by varying the concentration of the acetic acid modulator and the synthesis time, the linker vacancies can be tuned systematically, leading to dramatically enhanced porosity. We obtained samples with pore volumes ranging from 0.44 to 1.0 cm(3)/g and Brunauer-Emmett-Teller surface areas ranging from 1000 to 1600 m(2)/g, the largest values of which are ∼150% and ∼60% higher than the theoretical values of defect-free UiO-66 crystal, respectively. The linker vacancies also have profound effects on the gas adsorption behaviors of UiO-66, in particular CO2. Finally, comparing the gas adsorption of hydroxylated and dehydroxylated UiO-66, we found that the former performs systematically better than the latter (particularly for CO2) suggesting the beneficial effect of the -OH groups. This finding is of great importance because hydroxylated UiO-66 is the practically more relevant, non-air-sensitive form of this MOF. The preferred gas adsorption on the metal center was confirmed by neutron diffraction measurements, and the gas binding strength enhancement by the -OH group was further supported by our first-principles calculations.
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            Algorithms and tools for high-throughput geometry-based analysis of crystalline porous materials

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              • Article: not found

              Computation-Ready, Experimental Metal–Organic Frameworks: A Tool To Enable High-Throughput Screening of Nanoporous Crystals

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                Author and article information

                Journal
                Proc Natl Acad Sci U S A
                Proc. Natl. Acad. Sci. U.S.A
                pnas
                pnas
                PNAS
                Proceedings of the National Academy of Sciences of the United States of America
                National Academy of Sciences
                0027-8424
                1091-6490
                14 January 2020
                26 December 2019
                26 December 2019
                : 117
                : 2
                : 877-882
                Affiliations
                [1] aSchool of Chemical & Biomolecular Engineering, Georgia Institute of Technology , Atlanta, GA 30332-0100
                Author notes
                2To whom correspondence may be addressed. Email: david.sholl@ 123456chbe.gatech.edu .

                Edited by Alexis T. Bell, University of California, Berkeley, CA, and approved November 26, 2019 (received for review October 22, 2019)

                Author contributions: M.A. and D.S.S. designed research; M.A., R.H., and D.H. performed research; M.A. and R.H. analyzed data; and M.A. and D.S.S. wrote the paper.

                1M.A. and R.H. contributed equally to this work.

                Author information
                http://orcid.org/0000-0002-0331-5994
                http://orcid.org/0000-0002-2771-9168
                Article
                201918484
                10.1073/pnas.1918484117
                6969490
                31879338
                146272bf-4cd1-4fc4-b766-b4a19a9a6f2e
                Copyright © 2020 the Author(s). Published by PNAS.

                This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND).

                History
                Page count
                Pages: 6
                Funding
                Funded by: US Department of Energy Basic Energy Sciences
                Award ID: DE-SC0012577
                Award Recipient : Mayank Agrawal Award Recipient : Rebecca Han Award Recipient : Dinushka Herath Award Recipient : David Sholl
                Categories
                Physical Sciences
                Chemistry

                reproducibility,chemical synthesis,metal-organic frameworks

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