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Title: Chirality in adsorption on solid surfaces

Abstract

Chemical chirality on solid surfaces has important implications in analytical separations, selective crystallizations and catalysis, and may help explain the origin of homochirality in life.

Authors:
ORCiD logo [1]
  1. Department of Chemistry and UCR Center for Catalysis; University of California; Riverside; USA
Publication Date:
Research Org.:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1539896
DOE Contract Number:  
SC0008703
Resource Type:
Journal Article
Journal Name:
Chemical Society Reviews
Additional Journal Information:
Journal Volume: 46; Journal Issue: 23; Journal ID: ISSN 0306-0012
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
Chemistry

Citation Formats

Zaera, Francisco. Chirality in adsorption on solid surfaces. United States: N. p., 2017. Web. doi:10.1039/c7cs00367f.
Zaera, Francisco. Chirality in adsorption on solid surfaces. United States. doi:10.1039/c7cs00367f.
Zaera, Francisco. Sun . "Chirality in adsorption on solid surfaces". United States. doi:10.1039/c7cs00367f.
@article{osti_1539896,
title = {Chirality in adsorption on solid surfaces},
author = {Zaera, Francisco},
abstractNote = {Chemical chirality on solid surfaces has important implications in analytical separations, selective crystallizations and catalysis, and may help explain the origin of homochirality in life.},
doi = {10.1039/c7cs00367f},
journal = {Chemical Society Reviews},
issn = {0306-0012},
number = 23,
volume = 46,
place = {United States},
year = {2017},
month = {1}
}

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line-height:1.8em;"> <li> <span style="color:#7cb342;"> Bonalumi, Norberto; Vargas, Angelo; Ferri, Davide</span> </li> <li> Journal of the American Chemical Society, Vol. 127, Issue 23</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/ja050424z" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/ja050424z<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1007/s10562-006-0068-0" target="_blank" rel="noopener noreferrer" class="name">Kinetic Aspects of Nonlinear Phenomena in Heterogeneous Enantioselective Catalysis<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2006-07-01">July 2006</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Murzin, Dmitry Yu; Toukoniitty, Esa</span> </li> <li> Catalysis Letters, Vol. 109, Issue 3-4</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1007/s10562-006-0068-0" class="text-muted" target="_blank" rel="noopener noreferrer">10.1007/s10562-006-0068-0<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1002/anie.200705241" target="_blank" rel="noopener noreferrer" class="name">Nonlinear Effects in Asymmetric Catalysis<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2009-01-05">January 2009</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Satyanarayana, Tummanapalli; Abraham, Susan; Kagan, Henri B.</span> </li> <li> Angewandte Chemie International Edition, Vol. 48, Issue 3</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1002/anie.200705241" class="text-muted" target="_blank" rel="noopener noreferrer">10.1002/anie.200705241<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1007/s11144-011-0298-z" target="_blank" rel="noopener noreferrer" class="name">Unusual behavior of modifier mixtures in heterogeneous enantioselective catalysis: beyond nonlinear phenomena<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2011-03-20">March 2011</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Murzin, Dmitry Yu.; Szőllősi, György</span> </li> <li> Reaction Kinetics, Mechanisms and Catalysis, Vol. 103, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1007/s11144-011-0298-z" class="text-muted" target="_blank" rel="noopener noreferrer">10.1007/s11144-011-0298-z<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/j.catcom.2012.12.009" target="_blank" rel="noopener noreferrer" class="name">Modifier–substrate interactions of various types in the Orito reaction: Reversal of the enantioselection in the hydrogenation of ketopantolactone on Pt modified by β-isocinchonine and O-phenylcinchonidine<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2013-02-01">February 2013</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Szőllősi, György; Balázsik, Katalin; Bucsi, Imre</span> </li> <li> Catalysis Communications, Vol. 32</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/j.catcom.2012.12.009" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/j.catcom.2012.12.009<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/S1566-7367(02)00212-1" target="_blank" rel="noopener noreferrer" class="name">In-situ Raman investigation of cinchonidine adsorption on polycrystalline platinum in ethanol<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2002-12-01">December 2002</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Chu, Wei; LeBlanc, Rene J.; Williams, Christopher T.</span> </li> <li> Catalysis Communications, Vol. 3, Issue 12</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/S1566-7367(02)00212-1" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/S1566-7367(02)00212-1<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1021/la027031n" target="_blank" rel="noopener noreferrer" class="name">In Situ Characterization of Adsorbates in Solid−Liquid Interfaces by Reflection−Absorption Infrared Spectroscopy<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2003-04-01">April 2003</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Kubota, Jun; Ma, Zhen; Zaera, Francisco</span> </li> <li> Langmuir, Vol. 19, Issue 8</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/la027031n" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/la027031n<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1021/jp0753878" target="_blank" rel="noopener noreferrer" class="name">Enantiospecific Orientation of <em>R</em> –3-Methylcyclohexanone on the Chiral Cu(643) <sup> <em>R</em> / <em>S</em> </sup> Surfaces<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2008-04-29">April 2008</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Horvath, Joshua D.; Baker, Layton; Gellman, Andrew J.</span> </li> <li> The Journal of Physical Chemistry C, Vol. 112, Issue 20</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/jp0753878" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/jp0753878<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1007/s11244-011-9756-0" target="_blank" rel="noopener noreferrer" class="name">Enantiospecific Adsorption of (R)-3-Methylcyclohexanone on Naturally Chiral Surfaces Vicinal to Cu(110)<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2011-10-20">October 2011</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Huang, Ye; Gellman, Andrew J.</span> </li> <li> Topics in Catalysis, Vol. 54, Issue 19-20</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1007/s11244-011-9756-0" class="text-muted" target="_blank" rel="noopener noreferrer">10.1007/s11244-011-9756-0<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1039/b800411k" target="_blank" rel="noopener noreferrer" class="name">Chiral expression from molecular assemblies at metal surfaces: insights from surface science techniques<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2009-01-01">January 2009</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#7cb342;"> Raval, R.</span> </li> <li> Chemical Society Reviews, Vol. 38, Issue 3</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/b800411k" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/b800411k<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> </div> <div class="pagination-container small"> <a class="pure-button prev page" href="#" rel="prev"><span class="fa fa-angle-left"></span></a><ul class="pagination d-inline-block" style="padding-left:.2em;"></ul><a class="pure-button next page" href="#" rel="next"><span class="fa fa-angle-right"></span></a> </div> </div> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a href="" class="reference-type-filter tab-nav" data-tab="biblio-references" data-filter="type" data-pattern="*"><span class="fa fa-angle-right"></span> All References</a></li> <li class="small" style="margin-left:.75em; 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float:none;">[ × clear filter / sort ]</a> </div> </form> </div> </div> </div> </section> <section id="biblio-related" class="tab-content tab-content-sec " data-tab="biblio"> <div class="row"> <div class="col-sm-9 order-sm-9"> <section id="biblio-similar" class="tab-content tab-content-sec active" data-tab="related"> <div class="padding"> <p class="lead text-muted" style="font-size: 18px; margin-top:0px;">Similar records in OSTI.GOV collections:</p> <aside> <ul class="item-list" itemscope itemtype="http://schema.org/ItemList" style="padding-left:0; list-style-type: none;"> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="0" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1036747-molecular-level-design-heterogeneous-chiral-catalysis" itemprop="url">Molecular-Level Design of Heterogeneous Chiral Catalysis</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Technical Report</small><span class="authors"> <span class="author">Francisco Zaera</span> <span class="text-muted pubdata"></span> </span> </div> <div class="abstract">The following is a proposal to continue our multi-institutional research on heterogeneous chiral catalysis. Our team combines the use of surface-sensitive analytical techniques for the characterization of model systems with quantum and statistical mechanical calculations to interpret experimental data and guide the design of future research. Our investigation focuses on the interrelation among the three main mechanisms by which enantioselectivity can be bestowed to heterogeneous catalysts, namely: (1) by templating chirality via the adsorption of chiral supramolecular assemblies, (2) by using chiral modifiers capable of forming chiral complexes with the reactant and force enantioselective surface reactions, and (3) by forming<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> naturally chiral surfaces using imprinting chiral agents. Individually, the members of our team are leaders in these various aspects of chiral catalysis, but the present program provides the vehicle to generate and exploit the synergies necessary to address the problem in a comprehensive manner. Our initial work has advanced the methodology needed for these studies, including an enantioselective titration procedure to identify surface chiral sites, infrared spectroscopy in situ at the interface between gases or liquids and solids to mimic realistic catalytic conditions, and DFT and Monte Carlo algorithms to simulate and understand chirality on surfaces. The next step, to be funded by the monies requested in this proposal, is to apply those methods to specific problems in chiral catalysis, including the identification of the requirements for the formation of supramolecular surface structures with enantioselective behavior, the search for better molecules to probe the chiral nature of the modified surfaces, the exploration of the transition from supramolecular to one-to-one chiral modification, the correlation of the adsorption characteristics of one-to-one chiral modifiers with their physical properties, in particular with their configuration, and the development of ways to imprint chiral centers on achiral solid surfaces. Chiral catalysis is not only a problem of great importance in its own right, but also the ultimate test of how to control selectivity in catalysis. The time is ripe for fundamental work in heterogeneous chiral catalysis to provide the U.S. with a leadership role in developing the next generation of catalytic processes for medicinal and agrochemical manufacturing. Our team provides the required expertise for a synergistic and comprehensive integration of physical and chemical experimentation with solid state and molecular reactivity theories to solve this problem.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink">DOI: <a class="misc doi-link " href="https://doi.org/10.2172/1036747" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1036747" data-product-type="Technical Report" data-product-subtype="" >10.2172/1036747</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/servlets/purl/1036747" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1036747" data-product-type="Technical Report" data-product-subtype="" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="1" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/10192217-time-resolved-analytical-methods-liquid-solid-interfaces-progress-report-november-october" itemprop="url">Time-resolved analytical methods for liquid/solid interfaces. Progress report, November 1, 1993--October 31, 1994</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Technical Report</small><span class="authors"> <span class="author">Harris, J.M.</span> <span class="text-muted pubdata"></span> </span> </div> <div class="abstract">A number of chemical phenomena that occur at the boundaries between insulating solids and liquids (adsorption, partition, monolayer self-assembly, catalysis, and chemical reactions) are important to energy-related analytical chemistry. These phenomena are central to the development and understanding of chromatographic methods, solid-phase extraction techniques, immobilized analytical reagents, and optical sensors. The goal of this program, therefore, is to develop surface-sensitive spectroscopies by which chemical kinetics at liquid/solid interfaces can be observed on time-scales from nanoseconds to seconds. In the second year of this program, the authors have used temperature-jump relaxation measurements to monitor adsorption/desorption kinetics at liquid/solid interfaces using Joule<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> heating to compare the adsorption of ions from solution onto C1- and C4-derivatized silica surfaces. They completed a study of rate of migration of covalently-attached ligands on silica surfaces; from the temperature-dependence of the migration, the large energy barrier to migration was estimated. Surface heterogeneity of adsorption sites on silica was characterized by time-resolve fluorescence, and the chemical origins investigated by Si{sup 29} NMR spectroscopy. Surface-enhance Raman and fluorescence spectroscopies were modified to study adsorption and binding to silica surfaces. Molecular dynamics simulations were started to help better understand kinetic barriers to adsorption; ESR probe measurements were launched to measure and compare the chain mobility of silica-attached alkyl ligands.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink">DOI: <a class="misc doi-link " href="https://doi.org/10.2172/10192217" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="10192217" data-product-type="Technical Report" data-product-subtype="" >10.2172/10192217</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/servlets/purl/10192217" title="Link to document media" target="_blank" rel="noopener" data-ostiid="10192217" data-product-type="Technical Report" data-product-subtype="" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="2" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/7072749-adsorption-calorimetry-enhanced-oil-recovery" itemprop="url">Adsorption calorimetry in enhanced oil recovery</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Conference</small><span class="authors"> <span class="author">Noll, L.A.</span> <span class="text-muted pubdata"> - Am. Chem. Soc., Div. Pet. Chem., Prepr.; (United States)</span> </span> </div> <div class="abstract">Adsorption calorimetry is a technique which has been used at the National Institute for Petroleum and Energy Reserch (NIPER) to help in the understanding of adsorption as it impacts enhanced oil recovery by chemical flooding. Abstraction of chemicals by reservoir minerals comprises a major obstacle to the technical and economic success of this process. Adsorption is also important in other fields such as catalysis, lubrication, ore flotation, and printing. Adsorption calorimetry is useful because it measures both the amount of adsorption and its enthalpy. The enthalpy helps to guide the extrapolation of adsorption to higher temperatures as well as acting<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> as a probe of surface properties such as heterogeneity. Adsorption calorimetry helps to distinguish physical from chemisorption. It is also useful in distinguishing water-wet from oil-wet surfaces. This paper discusses flow adsorption calorimetry. The advantage of using a flowing system over the classic immersion technique is that it is fast and easy to use, and data for the entire isotherm are collected on a single sample of solid. In flow calorimetry the surface excess amount and the thermal data are obtained simultaneously on one and the same sample of solid, thus avoiding some sampling problems. Some disadvantages of the method are somewhat short equilibration times and the cumulative nature of the data. Aspects of adsorption of special interest to enhanced oil recovery such as the nature and charge of minerals, the structure and charge of surfactants, the effects of brine and temperature, and the effects of aqueous or hydrocarbon environment are important parameters of surfactant flooding; they are treated in this paper.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="3" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/451100-quest-chirality" itemprop="url">The quest for chirality</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Bonner, W.A.</span> <span class="text-muted pubdata"> - AIP Conference Proceedings</span> </span> </div> <div class="abstract">The indispensable role played by homochirality and chiral homogeneity in the self-replication of crucial biomolecules is stressed, with the conclusion that life could neither exist nor originate without these chiral molecular attributes. Hypotheses historically proposed for the origin of chiral molecules on Earth are reviewed, including biogenic theories as well as abiotic theories embracing both indeterminate and determinate mechanisms. Indeterminate mechanisms, including autocatalytic symmetry breaking, asymmetric adsorption on quartz and clay minerals, and asymmetric syntheses in chiral crystals, are discussed and evaluated in the context of the prebiotic environment. Abiotic determinate mechanisms based on electric, magnetic and gravitational fields, on<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> circularly polarized light (CPL), and on parity violation effects are summarized, with the emphasis that only CPL has proved practicable experimentally, but that it would be implausible on the primitive Earth. Mechanisms for the amplification of small, indigenous enantiomeric excesses are discussed, with one involving the partial polymerization of amino acids and the partial hydrolysis of polypeptides suggested as potentially viable prebiotically. Aspects of the turbulent, chirality-destructive primeval environment are described, with the conclusion that all of the above mechanisms for the {ital terrestrial} prebiotic origin of chirality would be non-viable, and that an alternative extraterrestrial source for the accumulation of chiral molecules on primitive Earth must have been operative. A scenario for this is outlined, in which we postulate that asymmetric photolysis of the organic mantles on interstellar grains in molecular clouds by circularly polarized ultraviolet synchrotron radiation from the neutron star remnants of supernovae produces chiral molecules in the grain mantles. (Abstract Truncated)</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink">DOI: <a class="misc doi-link " href="https://doi.org/10.1063/1.51234" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="451100" data-product-type="Journal Article" data-product-subtype="AC" >10.1063/1.51234</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="4" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1479978-probing-energetics-moleculematerial-interactions-interfaces-nanopores" itemprop="url">Probing the Energetics of Molecule–Material Interactions at Interfaces and in Nanopores</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Li, Gengnan</span> ; <span class="author">Sun, Hui</span> ; <span class="author">Xu, Hongwu</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Journal of Physical Chemistry. C</span> </span> </div> <div class="abstract">During the past decades, advances in interfacial chemistries at the molecular level are shaping our world by playing crucial roles in balancing global scale energy crisis and critical environmental concerns. However, systematic investigations into the binding energies, site distribution and their correlation with the molecular-level surface assemblages and structures at interfaces and in nanopores are rarely documented. In this review, we summarize a set of systematic calorimetric studies on surface energetics we performed during the last decade. These studies demonstrate how thermochemistry can reveal crucial energetic insights into a series of molecule – material interactions relevant to a number of<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> applications, including carbon capture and sequestration, energy production, sustainable chemical processing, catalysis, and nanogeoscience. Calorimetric methodologies developed and applied include direct gas adsorption calorimetry, nearroom temperature solvent immersion/solution calorimetry and high temperature oxide melt solution calorimetry. Using these highly unique techniques, we reveal the thermodynamic complexity of carbon dioxide capture on metal – organic framework (MOF) sorbents with built-in and grafted nucleophilic functional groups (-OH and -NH2). These studies suggest that carbon dioxide adsorption on functionalized MOFs is a complex process involving multiple thermodynamic factors, as reflected by changes in surface phase and structure, chemical bonding and degree of disorder with varying temperature and gas loading. The fundamental insights obtained may help optimize the design, synthesis and application of MOF-based carbon dioxide sorbents for carbon capture and sequestration. In parallel, we also explore the energetics of interaction and competition between small molecules (water, carbon dioxide, methane, simple and complex organics) and inorganic materials (calcite, silica, zirconia, zeolites, mesoporous frameworks, alumina, and uranium), at interfaces and in nanopores. Combined with spectroscopic, diffraction, electron microscopic and computational techniques, the energetics of gas/liquid – solid interactions can be correlated with specific bonds, molecular configurations and nanostructures. Although the energetics evolves continuously from weak association to strong bonding to classical capping, distinct regions of rapidly changing stepwise energetics often separate the different regimes. These phenomena are closely related to the properties of inorganic material surfaces (hydrophobicity and acidity/basicity), the framework architectures, and the chemical nature of adsorbate molecules. These direct thermodynamic insights reinforce our understanding of complex small molecule – inorganic material interactions important to multiple disciplines of chemical engineering, materials science, nanogeoscience and environmental technology, including heterogeneous catalysis, molecular separation, material design and synthesis, biomineralization, contaminant and nutrient transport, carbonate formation, and water – organic competitions on material/mineral surfaces.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <span class="fa fa-book text-muted" aria-hidden="true"></span> Cited by 1<div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/acs.jpcc.7b07450" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1479978" data-product-type="Journal Article" data-product-subtype="AM" >10.1021/acs.jpcc.7b07450</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/servlets/purl/1479978" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1479978" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> </ul> </aside> </div> </section> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a class="tab-nav disabled" data-tab="related" style="color: #636c72 !important; opacity: 1;"><span class="fa fa-angle-right"></span> Similar Records</a></li> </ul> </div> </div> </section> </div></div> </div> </div> </section> <footer class="" style="background-color:#f9f9f9; /* padding-top: 0.5rem; */"> <div class="footer-minor"> <div class="container"> <hr class="footer-separator" /> <div class="text-center" style="margin-top:1.25rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list" id="footer-org-menu"> <li class="pure-menu-item d-block d-inline-small"> <a href="https://energy.gov" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-us-doe-min" alt="U.S. Department of Energy" /> </a> </li> <li class="pure-menu-item d-block d-inline-small"> <a href="https://www.energy.gov/science/office-science" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-office-of-science-min" alt="Office of Science" /> </a> </li> <li class="pure-menu-item d-block d-inline-small"> <a href="/"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-osti-min" alt="Office of Scientific and Technical Information" /> </a> </li> </ul> </div> </div> <div class="text-center small" style="margin-top:0.5em;margin-bottom:2.0rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list"> <li class="pure-menu-item"><a href="/disclaim" class="pure-menu-link"><span class="fa fa-institution"></span> Website Policies <span class="d-none d-sm-inline" style="color:#737373;">/ Important Links</span></a></li> <li class="pure-menu-item"><a href="/contact" class="pure-menu-link"><span class="fa fa-comments-o"></span> Contact Us</a></li> <li class="d-block d-md-none mb-1"></li> <li class="pure-menu-item"><a href="https://www.facebook.com/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-facebook" style=""></span></a></li> <li class="pure-menu-item"><a href="https://twitter.com/OSTIgov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-twitter" style=""></span></a></li> <li class="pure-menu-item"><a href="https://www.youtube.com/user/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-youtube-play" style=""></span></a></li> </ul> </div> </div> </div> </div> </footer> <link href="/css/ostigov.fonts.191107.1502.css" rel="stylesheet"> <script src="/js/ostigov.191107.1502.js"></script><noscript></noscript> <script defer src="/js/ostigov.biblio.191107.1502.js"></script><noscript></noscript> <script defer src="/js/lity.js"></script><noscript></noscript> <script async type="text/javascript" src="/js/Universal-Federated-Analytics-Min.js?agency=DOE" id="_fed_an_ua_tag"></script><noscript></noscript> </body> <!-- OSTI.GOV v.191107.1502 --> </html>