Faraday Discussions最新文献

{"title":"Mixed quantum/classical theory (MQCT) approach to the dynamics of molecule–molecule collisions in complex systems†","authors":"Carolin Joy, Bikramaditya Mandal, Dulat Bostan, Marie-Lise Dubernet and Dmitri Babikov","doi":"10.1039/D3FD00166K","DOIUrl":"10.1039/D3FD00166K","url":null,"abstract":"<p >We developed a general theoretical approach and a user-ready computer code that permit study of the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule–molecule collisions. The method is a mixture of classical and quantum mechanics. The internal ro-vibrational motion of collision partners is treated quantum mechanically using a time-dependent Schrödinger equation that captures many quantum phenomena including state quantization and zero-point energy, propensity and selection rules for state-to-state transitions, quantum symmetry and interference phenomena. A significant numerical speed up is obtained by describing the translational motion of collision partners classically, using the Ehrenfest mean-field trajectory approach. Within this framework a family of approximate methods for collision dynamics is developed. Several benchmark studies for diatomic and triatomic molecules, such as H<small>₂</small>O and ND<small>₃</small> collided with He, H<small>₂</small> and D<small>₂</small>, show that the results of MQCT are in good agreement with full-quantum calculations in a broad range of energies, especially at high collision energies where they become nearly identical to the full quantum results. Numerical efficiency of the method and massive parallelism of the MQCT code permit us to embrace some of the most complicated collisional systems ever studied, such as C<small>₆</small>H<small>₆</small> + He, CH<small>₃</small>COOH + He and H<small>₂</small>O + H<small>₂</small>O. Application of MQCT to the collisions of chiral molecules such as CH<small>₃</small>CHCH<small>₂</small>O + He, and to molecule–surface collisions is also possible and will be pursued in the future.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 225-248"},"PeriodicalIF":3.4,"publicationDate":"2024-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141069804","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Exploring the chemical dynamics of phenanthrene (C14H10) formation via the bimolecular gas-phase reaction of the phenylethynyl radical (C6H5CC) with benzene (C6H6)†","authors":"Shane J. Goettl, Zhenghai Yang, Chao He, Ankit Somani, Adrian Portela-Gonzalez, Wolfram Sander, Alexander M. Mebel and Ralf I. Kaiser","doi":"10.1039/D3FD00159H","DOIUrl":"10.1039/D3FD00159H","url":null,"abstract":"<p >The exploration of the fundamental formation mechanisms of polycyclic aromatic hydrocarbons (PAHs) is crucial for the understanding of molecular mass growth processes leading to two- and three-dimensional carbonaceous nanostructures (nanosheets, graphenes, nanotubes, buckyballs) in extraterrestrial environments (circumstellar envelopes, planetary nebulae, molecular clouds) and combustion systems. While key studies have been conducted exploiting traditional, high-temperature mechanisms such as the hydrogen abstraction–acetylene addition (HACA) and phenyl addition–dehydrocyclization (PAC) pathways, the complexity of extreme environments highlights the necessity of investigating chemically diverse mass growth reaction mechanisms leading to PAHs. Employing the crossed molecular beams technique coupled with electronic structure calculations, we report on the gas-phase synthesis of phenanthrene (C<small>₁₄</small>H<small>₁₀</small>)—a three-ring, 14π benzenoid PAH—<em>via</em> a phenylethynyl addition–cyclization–aromatization mechanism, featuring bimolecular reactions of the phenylethynyl radical (C<small>₆</small>H<small>₅</small>CC, X<small>²</small>A<small>₁</small>) with benzene (C<small>₆</small>H<small>₆</small>) under single collision conditions. The dynamics involve a phenylethynyl radical addition to benzene without entrance barrier leading eventually to phenanthrene <em>via</em> indirect scattering dynamics through C<small>₁₄</small>H<small>₁₁</small> intermediates. The barrierless nature of reaction allows rapid access to phenanthrene in low-temperature environments such as cold molecular clouds which can reach temperatures as low as 10 K. This mechanism constitutes a unique, low-temperature framework for the formation of PAHs as building blocks in molecular mass growth processes to carbonaceous nanostructures in extraterrestrial environments thus affording critical insight into the low-temperature hydrocarbon chemistry in our universe.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 509-522"},"PeriodicalIF":3.4,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141064492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dynamics of carbene formation in the reaction of methane with the tantalum cation in the gas phase†","authors":"Marcel Meta, Maximilian E. Huber, Maurice Birk, Martin Wedele, Milan Ončák and Jennifer Meyer","doi":"10.1039/D3FD00171G","DOIUrl":"10.1039/D3FD00171G","url":null,"abstract":"<p >The controlled activation of methane has drawn significant attention throughout various disciplines over the last few decades. In gas-phase experiments, the use of model systems with reduced complexity compared to condensed-phase catalytic systems allows us to investigate the intrinsic reactivity of elementary reactions down to the atomic level. Methane is rather inert in chemical reactions, as the weakening or cleavage of a C–H bond is required to make use of methane as C<small>₁</small>-building block. The simplest model system for transition-metal-based catalysts is a mono-atomic metal ion. Only a few atomic transition-metal cations activate methane at room temperature. One of the most efficient elements is tantalum, which forms a carbene and releases molecular hydrogen in the reaction with methane: Ta<small>⁺</small> + CH<small>₄</small> → TaCH<small>₂</small><small>⁺</small> + H<small>₂</small>. The reaction takes place at room temperature due to efficient intersystem crossing from the quintet to the triplet surface, <em>i.e.</em>, from the electronic ground state of the tantalum cation to the triplet ground state of the tantalum carbene. This multi-state reactivity is often seen for reactions involving transition-metal centres, but leads to their theoretical treatment being a challenge even today. Chemical reactions, or to be precise reactive collisions, are dynamic processes making their description even more of a challenge to experiment and theory alike. Experimental energy- and angle-differential cross sections allow us to probe the rearrangement of atoms during a reactive collision. By interpreting the scattering signatures, we gain insight into the atomistic mechanisms and can move beyond stationary descriptions. Here, we present a study combining collision energy dependent experimentally measured differential cross sections with <em>ab initio</em> calculations of the minimum energy pathway. Product ion velocity distributions were recorded using our crossed-beam velocity map imaging experiment dedicated to studying transition-metal ion molecule reactions. TaCH<small>₂</small><small>⁺</small> velocity distributions reveal a significant degree of indirect dynamics. However, the scattering distributions also show signatures of rebound dynamics. We compare the present results to the oxygen transfer reaction between Ta<small>⁺</small> and carbon dioxide, which we recently studied.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 587-603"},"PeriodicalIF":3.4,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d3fd00171g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141064490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Bimolecular collision outcomes on multidimensional potential energy surfaces: infrared spectroscopy and activation of NO–alkane collision complexes","authors":"John P. Davis, P. Garrett Burroughs, W. Churchill Wilkinson, Ellora Majumdar and Nathanael M. Kidwell","doi":"10.1039/D3FD00176H","DOIUrl":"10.1039/D3FD00176H","url":null,"abstract":"<p >In bimolecular collisions between open-shell radicals and increasingly-larger alkanes, the relative impact configurations open the possibility of reactive and nonreactive outcomes that are isomer specific. To model the interaction potential between molecular scattering partners, observables are needed from experiments that can quantify both the initial molecular orientations and internal energies on multidimensional potential energy surfaces. Recent work by our group demonstrated that upon infrared (IR) excitation, the dynamics of the nitric oxide–methane collision complex (NO–CH<small>₄</small>) are dependent on the initial monomer geometries, as small changes in configuration substantially affect the energies, electronic couplings, and predissociation pathways due to the Jahn–Teller effect. This study focuses on the isomer-specific scattering mechanisms between NO and ethane (C<small>₂</small>H<small>₆</small>), encoded in the spectroscopic and dynamical signatures of the NO–C<small>₂</small>H<small>₆</small> collision complex. IR action spectroscopy with 1 + 1 resonance-enhanced multiphoton ionization of NO products was employed to characterize the fundamental CH stretch transitions of NO–C<small>₂</small>H<small>₆</small>, as well as to initiate the nonreactive decay mechanisms of the complex. Furthermore, velocity map imaging (VMI) was utilized to explore the dynamics prior to and following IR excitation of NO–C<small>₂</small>H<small>₆</small>, imprinted on the NO photoproducts. This work compares the dynamics from NO–C<small>₂</small>H<small>₆</small> and NO–CH<small>₄</small> vibrational predissociation, in which substantial differences are observed in the energy exchange mechanisms during the evolution of the collision complexes to products.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 262-278"},"PeriodicalIF":3.4,"publicationDate":"2024-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141064489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"An engineered T7 RNA polymerase for efficient co-transcriptional capping with reduced dsRNA byproducts in mRNA synthesis†","authors":"Mathew Miller, Oscar Alvizo, Scott Baskerville, Avinash Chintala, Chinping Chng, Justin Dassie, Jonathan Dorigatti, Gjalt Huisman, Stephan Jenne, Supriya Kadam, Neil Leatherbury, Stefan Lutz, Melissa Mayo, Arpan Mukherjee, Antoinette Sero, Stuart Sundseth, Jonathan Penfield, James Riggins and Xiyun Zhang","doi":"10.1039/D4FD00023D","DOIUrl":"10.1039/D4FD00023D","url":null,"abstract":"<p >Messenger RNA (mRNA) therapies have recently gained tremendous traction with the approval of mRNA vaccines for the prevention of SARS-CoV-2 infection. However, manufacturing challenges have complicated large scale mRNA production, which is necessary for the clinical viability of these therapies. Not only can the incorporation of the required 5′ 7-methylguanosine cap analog be inefficient and costly, <em>in vitro</em> transcription (IVT) using wild-type T7 RNA polymerase generates undesirable double-stranded RNA (dsRNA) byproducts that elicit adverse host immune responses and are difficult to remove at large scale. To overcome these challenges, we have engineered a novel RNA polymerase, T7-68, that co-transcriptionally incorporates both di- and tri-nucleotide cap analogs with high efficiency, even at reduced cap analog concentrations. We also demonstrate that IVT products generated with T7-68 have reduced dsRNA content.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"252 ","pages":" 431-449"},"PeriodicalIF":3.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d4fd00023d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141064164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Six-dimensional quantum dynamics of an Eley–Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111)","authors":"Longlong Xiong, Liang Zhang, Bin Zhao and Bin Jiang","doi":"10.1039/D3FD00163F","DOIUrl":"10.1039/D3FD00163F","url":null,"abstract":"<p >In the form of direct abstraction of a surface adsorbate by a gaseous projectile, the Eley–Rideal (ER) reaction at the gas–surface interface manifests interesting dynamics. Unfortunately, high-dimensional quantum dynamical (QD) studies for ER reactions remain very challenging, which demands a large configuration space and the coordinate transformation of wavefunctions. Here, we report the first six-dimensional (6D) fully coupled quantum scattering method for studying the ER reaction between gas phase H(D) atoms and adsorbed D(H) atoms on a rigid Cu(111) surface. Reaction probabilities and product rovibrational state distributions obtained by this 6D model are found to be quite different from those obtained by reduced-dimensional QD models, demonstrating the high-dimensional nature of the ER reaction. Using two distinct potential energy surfaces (PESs), we further discuss the influence of the PES on the calculated product vibrational and rotational state distributions, in comparison with experimental results. The lateral corrugation and the exothermicity of the PES are found to play a critical role in controlling the energy disposal in the ER reaction.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 457-470"},"PeriodicalIF":3.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d3fd00163f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140955242","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Molecular beam scattering of ammonia from a dodecane flat liquid jet","authors":"Steven Saric, Walt Yang and Daniel M. Neumark","doi":"10.1039/D3FD00169E","DOIUrl":"10.1039/D3FD00169E","url":null,"abstract":"<p >The evaporation and scattering of ND<small>₃</small> from a dodecane flat liquid jet are investigated and the results are compared with previous studies on molecular beam scattering from liquid surfaces. Evaporation is well-described by a Maxwell–Boltzmann flux distribution with a cos <em>θ</em> angular distribution at the liquid temperature. Scattering experiments at <em>E</em><small>_i</small> = 28.8 kJ mol<small>⁻¹</small> over a range of deflection angles show evidence for impulsive scattering and thermal desorption. At a deflection angle of 90°, the thermal desorption fraction is 0.49, which is higher than that of other molecules previously scattered from dodecane and consistent with work performed on NH<small>₃</small> scattering from a squalane-wetted wheel. ND<small>₃</small> scattering from dodecane results in super-specular scattering, as seen in previous experiments on dodecane. The impulsive scattering channel is fitted to a “soft-sphere” model, yielding an effective surface mass of 55 amu and an internal excitation of 5.08 kJ mol<small>⁻¹</small>. Overall, impulsively scattered ND<small>₃</small> behaves similarly to other small molecules scattered from dodecane.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"251 ","pages":" 382-394"},"PeriodicalIF":3.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140955238","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Investigating the effect of fusion partners on the enzymatic activity and thermodynamic stability of poly(ethylene terephthalate) degrading enzymes†","authors":"Liliana Oliveira, Alex Cahill, Len Wuscher, Kerry R. Green, Victoria Bemmer and Bruce R. Lichtenstein","doi":"10.1039/D4FD00067F","DOIUrl":"10.1039/D4FD00067F","url":null,"abstract":"<p >Plastics are a cornerstone of the modern world, yet the durable material properties that we have come to depend upon have made them recalcitrant environmental pollutants. Biological solutions in the form of engineered enzymes offer low energy and sustainable approaches to recycle and upcycle plastic waste, uncoupling their production and end of life from fossil fuels and greenhouse gases. These enzymes however, encounter immense challenges acting on plastics: facing hydrophobic surfaces, molecular crowding, and high levels of substrate heterogeneity. There have been mixed reports about the benefits of fusing partner domains to polyethylene terephthalate (PET) degrading enzymes, with moderate improvements identified under specific conditions, but no clarity into the factors that underlie the mechanisms. Here, we use the SpyCatcher003:SpyTag003 technology, which demonstrates a profound 47 °C shift in <em>T</em><small>_m</small> upon irreversible complex formation, to investigate the influence of the thermal stability of the fusion partner on a range of PETases selected for their optimal reaction temperatures. We find that the thermal stability of the fusion partner does not have a positive correlation on the activity of the enzymes or their evident kinetic and thermal stabilities. Instead, it appears that the fusion to less stable SpyCatcher003 tends to increase the measured activation energy of unfolding compared to the more stable complex and wildtype enzymes. Despite this, the fusions to SpyCatcher003 do not show significantly better catalytic activity on PET films, with or without SpyTag003, and were found to be sometimes disruptive. The approach we highlight here, in using a fusion partner with controllable melting temperature, allowed us to dissect the impact of the stability of a fusion partner on enzyme properties. Although fusion stability did not appear to be coupled with identifiable trends in enzymatic activities, careful analysis of the unfolding pathways, and solid and solution activities of a wider range of enzymes may yield a more detailed understanding.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"252 ","pages":" 468-479"},"PeriodicalIF":3.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d4fd00067f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141064011","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ion transport in polymerized ionic liquids: a comparison of polycation and polyanion systems","authors":"Javad Jeddi, Jukka Niskanen, Benoît H. Lessard and Joshua Sangoro","doi":"10.1039/D4FD00070F","DOIUrl":"10.1039/D4FD00070F","url":null,"abstract":"<p >The correlation among chemical structure, mesoscale structure, and ion transport in 1,2,3-triazole-based polymerized ionic liquids (polyILs) featuring comparable polycation and polyanion backbones is investigated by wide-angle X-ray scattering (WAXS), differential scanning calorimetry, and broadband dielectric spectroscopy (BDS). Above the glass transition temperature, <em>T</em><small>_g</small>, higher ionic conductivity is observed in polycation polyILs compared to their polyanion counterparts, and ion conduction is enhanced by increasing the counterion volume in both polycation or polyanion polyILs. Below <em>T</em><small>_g</small>, polyanions show lower activation energy associated with ion conduction. However, the validity of the Barton–Nakajima–Namikawa relation indicates that hopping conduction is the dominant charge transport mechanism in all the polyILs studied. While a significant transition from a Vogel–Fulcher–Tammann to Arrhenius type of thermal activation is observed below <em>T</em><small>_g</small>, the decoupling index, often used to quantify the extent to which segmental dynamics and ion conduction are correlated, remains unaltered for the polyILs studied, suggesting that this index may not be a general parameter to characterize charge transport in polymerized ionic liquids. Furthermore, detailed analyses of the WAXS results indicate that both the mobile ion type and the structure of the pendant groups control mesoscale organization. These findings are discussed within the framework of recent models, which account for the subtle interplay between electrostatic and elastic forces in determining ion transport in polyILs. The findings demonstrate the intricate balance between the chemical structure and interactions in polyILs that determine ion conduction in this class of polymer electrolytes.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"253 ","pages":" 426-440"},"PeriodicalIF":3.4,"publicationDate":"2024-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d4fd00070f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141061920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Striking the right balance of encoding electron correlation in the Hamiltonian and the wavefunction ansatz","authors":"Kalman Szenes, Maximilian Mörchen, Paul Fischill and Markus Reiher","doi":"10.1039/D4FD00060A","DOIUrl":"10.1039/D4FD00060A","url":null,"abstract":"<p >Multi-configurational electronic structure theory delivers the most versatile approximations to many-electron wavefunctions, flexible enough to deal with all sorts of transformations, ranging from electronic excitations, to open-shell molecules and chemical reactions. Multi-configurational models are therefore essential to establish universally applicable, predictive <em>ab initio</em> methods for chemistry. Here, we present a discussion of explicit correlation approaches which address the nagging problem of dealing with static and dynamic electron correlation in multi-configurational active-space approaches. We review the latest developments and then point to their key obstacles. Our discussion is supported by new data obtained with tensor network methods. We argue in favor of simple electron-only correlator expressions that may allow one to define transcorrelated models in which the correlator does not bear a dependence on molecular structure.</p>","PeriodicalId":49075,"journal":{"name":"Faraday Discussions","volume":"254 ","pages":" 359-381"},"PeriodicalIF":3.4,"publicationDate":"2024-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/fd/d4fd00060a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140833916","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}