Journal of the American Chemical Society最新文献

{"title":"HydE Catalytic Mechanism Is Powered by a Radical Relay with Redox-Active Fe(I)-Containing Intermediates.","authors":"Nanhao Chen, Guodong Rao, Lizhi Tao, R David Britt, Lee-Ping Wang","doi":"10.1021/jacs.4c12668","DOIUrl":"10.1021/jacs.4c12668","url":null,"abstract":"<p><p>[FeFe]-hydrogenases are enzymes that catalyze the redox interconversion of H⁺ and H₂ using a six-iron active site, known as the H-cluster, which consists of a structurally unique [2Fe]_<i>H</i> subcluster linked to a [4Fe-4S]_<i>H</i> subcluster. A set of enzymes, HydG, HydE, and HydF, are responsible for the biosynthesis of the [2Fe]_<i>H</i> subcluster. Among them, it is well established that HydG cleaves tyrosine into CO and CN^- and forms a mononuclear [Fe(II)(Cys)(CO)₂(CN)] complex. Recent work using EPR spectroscopy and X-ray crystallography show that HydE uses this organometallic Fe complex as its native substrate. The low spin Fe(II) center is reduced into an adenosylated Fe(I) species, which is proposed to form an Fe(I)Fe(I) dimer within HydE. The highly unusual transformation catalyzed by HydE draws interest in both biochemistry and organometallic chemistry. Due to the instability of the substrate, the intermediates, and the proposed product, experimental characterization of the detailed HydE mechanism and its final product is challenging. Herein, the catalytic mechanism of HydE is studied using hybrid quantum mechanics/molecular mechanics (QM/MM) molecular dynamics simulations. A radical relay mechanism was found for the cleavage of the cysteine S-Cβ bond that is energetically favored with respect to a closed-shell mechanism involving unconventional proton transfer. In addition, we propose a pathway for the dimerization of two Fe(I) complexes within the HydE hydrophobic cavity, which is consistent with the recent experimental result that HydF can perform [FeFe]-hydrogenase maturation with a synthetic dimer complex as the substrate. These simulation results take us further down the path to a more complete understanding of these enzymes that synthesize one of Nature's most efficient energy conversion catalysts.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"4800-4809"},"PeriodicalIF":14.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11826987/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Reactions of SleC, Its Structure and Inhibition in Mitigation of Spore Germination in <i>Clostridioides difficile</i>.","authors":"Choon Kim, Rafael Molina, Mijoon Lee, Alba Garay-Alvarez, Jingdong Yang, Yuanyuan Qian, Biruk T Birhanu, Dusan Hesek, Juan A Hermoso, Mayland Chang, Shahriar Mobashery","doi":"10.1021/jacs.4c14976","DOIUrl":"10.1021/jacs.4c14976","url":null,"abstract":"<p><p>Spore germination in <i>Clostridioides difficile</i> is initiated by a cascade of activities of several proteins that culminates in the activation of SleC, a cell-wall-processing enzyme. We report herein the details of the enzymatic activities of SleC by the use of synthetic peptidoglycan fragments and of spore sacculi. The reactions include the formation of 1,6-anhydromuramate─a hallmark of lytic transglycosylase activity─as well as a muramate hydrolytic product, both of which proceed through the same transient oxocarbenium species. Furthermore, we report the first X-ray structure of zymogenic prepro-SleC at 2.1 Å resolution. Additionally, the structure provides insights into the YabG and CspB cleavage sites necessary for the activation of the zymogen. The active site of SleC presents relevant differences in contrast to SpoIID, a homologous lytic transglycosylase involved in the sporulation <i>Clostridioides</i> species, explaining the ability of SleC to turn over the spore sacculus, a prerequisite for the germination event. A screening of an in-house library of compounds led to the discovery of an oxadiazole that binds to the mature (activated) form of SleC, whereby it shuts down the ability of spores to germinate in the presence of germinants. This is consistent with the SleC activity as an end-point for the germination cascade. The mechanistic knowledge and the inhibitor hold the promise in addressing an unmet medical need in intervention of recurrent infections by <i>C. difficile</i>.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":"5060-5070"},"PeriodicalIF":14.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062436","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ferrocyanide “Skin”-Mediated Anticatalysis: Mitigating Self-Discharge in Aqueous Electrochemical Devices","authors":"Jin Li, Shuo Sun, Hao Huang, Teng Zhai, Yanchen Liu, Minghui Gu, Hongye Yang, Mingqing Sun, Tianyi Kou, Shuang Li, Hui Xia","doi":"10.1021/jacs.4c16996","DOIUrl":"https://doi.org/10.1021/jacs.4c16996","url":null,"abstract":"The interest in aqueous energy storage devices is surging due to their exceptional safety profile. However, in aqueous energy storage systems, interfacial side reactions, predominantly attributed to the oxygen evolution reaction (OER), result in significant self-discharge, which is concomitant with the deterioration of both voltage and capacity. Herein, we propose the construction of a ferrocyanide “skin” on transition metal compounds (TMCs) to mitigate this issue. This engineered “skin” creates Fe–C≡N terminations, initiating a new reaction pathway featured by the bonding process of N–O and N–H bonds. This reaction pathway presents a significant energy barrier, effectively shielding the active sites for the OER from H₂O molecules and hydroxyl ions. Taking NiO as an example, the ferrocyanide “skin” effectively suppresses the undesired phase transition from NiOOH to Ni(OH)₂ during the idling process of a fully charged electrode, enabling the as-modified electrode to achieve a remarkable voltage retention of 80.0% after 1 week of idling within a device. Furthermore, this concept demonstrates extensive applicability, extending to a range of TMC materials, including but not limited to manganese oxide, vanadium oxide, and nickel cobalt oxide. These findings highlight the efficacy of the ferrocyanide “skin” design strategy as a broadly applicable paradigm for suppressing H₂O-induced undesirable phase transitions in aqueous energy storage devices.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"62 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401902","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Single-Enzyme Conversion of Tryptophan to Skatole and Cyanide Expands the Mechanistic Competence of Diiron Oxidases","authors":"Sanjoy Adak, Logan A. Calderone, August Krueger, Maria-Eirini Pandelia, Bradley S. Moore","doi":"10.1021/jacs.4c14573","DOIUrl":"https://doi.org/10.1021/jacs.4c14573","url":null,"abstract":"Skatole is a pungent heterocyclic compound derived from the essential amino acid <span>l</span>-tryptophan by bacteria in the mammalian digestive tract. The four-step anaerobic conversion of tryptophan to skatole is well-established; though, to date, no aerobic counterpart has been reported. Herein, we report the discovery of the oxygen-dependent skatole synthase SktA that single-handedly converts 5-bromo-<span>l</span>-tryptophan to 5-bromoskatole, obviating the need for a multienzyme process. SktA is part of a three-gene biosynthetic gene cluster (BGC) in the cyanobacterium <i>Nostoc punctiforme</i> NIES-2108 and functions as a nonheme diiron enzyme belonging to the heme oxygenase-like domain-containing oxidase (HDO) superfamily. Our detailed biochemical analyses revealed cyanide and bicarbonate as biosynthetic coproducts, while stopped-flow experiments showed the hallmark formation of a substrate-triggered peroxo Fe₂(III) intermediate. Overall, this work unravels an alternative pathway for converting tryptophan to skatole while also expanding the functional repertoire of HDO enzymes.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"13 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143401987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Single-Molecule-Sensitive Three-Dimensional Atomic Heterostructures with Extreme Light-Matter Coupling","authors":"Yi-Jui Yeh, Shao-Yu Chen, Wesley Wei-Wen Hsiao, Yoshifumi Oshima, Mari Takahashi, Shinya Maenosono, Kuo-Lun Tung, Wei-Hung Chiang","doi":"10.1021/jacs.4c15029","DOIUrl":"https://doi.org/10.1021/jacs.4c15029","url":null,"abstract":"Three-dimensional heterostructures (3DHS) with controlled compositions and tuned properties are highly desired for fundamental studies and applications in optoelectronics, nanocatalysis, clean energy, and biomedicine. However, conventional nanostructure engineering is hindered by challenges such as poor structural control, time- and energy-intensive processes, the use of hazardous and expensive chemicals, and harsh conditions. Here, we report plasma-assisted epitaxy (PAE) engineering of a metal–organic 3DHS with extreme light-matter interaction for rapid single-molecule-level sensing. Plasmonic-active 3DHS composed of structure-tuned gold–silver core–shell nanoparticles (AuAgCSNPs) was precisely engineered using stable and scalable microplasma-enabled nanofabrication under ambient conditions. The engineered AuAgCSNP-based 3DHS possessed exceptional Raman enhancement under suitable laser excitation, leading to single-molecule detection of SARS-CoV-2 spike proteins in simulated human saliva via surface-enhanced Raman scattering (SERS). The developed plasma fabrication method allows the production of centimeter-scale SERS-active metal–organic 3DHS on disposable, flexible, lightweight, and cost-effective substrates, thereby opening a new avenue for next-generation biosensing, nanoelectronics, nanocatalysis, and biomedical applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"59 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393864","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Synthesis and Reactivity of an Iron–Tin Complex with Adjacent Stannylidyne and Ferriostannylene Units","authors":"Yang Liu, Franz F. Westermair, Isabelle Becker, Sebastian Hauer, Michael Bodensteiner, Christoph Hennig, Gábor Balázs, Franc Meyer, Ruth M. Gschwind, Robert Wolf","doi":"10.1021/jacs.4c18423","DOIUrl":"https://doi.org/10.1021/jacs.4c18423","url":null,"abstract":"Heavier transition metal carbyne analogs hold significant potential for cooperative activation of small molecules. However, complexes containing more than one heavier tetrylidyne ligand RE (E = Si, Ge, Sn, Pb) are rare due to the high oligomerization tendency of RE ligands. In this study, we describe the complex [Fe(SnAr’)₂] (<b>1</b>; Ar’ = 2,6-Dipp₂-C₆H₃, Dipp = 2,6-<i>ⁱ</i>Pr₂–C₆H₃), which features adjacent Fe–Sn single and double bonds. Complex <b>1</b> exhibits versatile reactivity with transition metal and main group compounds. Treatment of complex <b>1</b> with Ni(COD)₂ (COD = 1,5-cyclooctadiene) yields the tetranuclear complex [Fe(μ-SnAr’)₂Ni] (<b>2</b>), characterized by an unusual “push–pull” interaction between nickel(0) and the two coordinating Sn atoms, as revealed by quantum chemical studies. The reaction of complex <b>1</b> with AlBr₃ results in Al–Br bond cleavage and Ar’ migration to aluminum. CH₃I adds oxidatively to the Sn atom that is singly bonded to Fe, while PMe₃ coordinates to Fe, inducing reversible cleavage of the Fe═Sn double bond. In addition, complex <b>1</b> activates inorganic molecules. CO₂ undergoes disproportionation to produce a carbonate-bridged Ar’Sn(μ–OCO₂)SnAr’ ligand, whereas CS₂ is reductively coupled to form an ethylene tetrathiolate ligand ([C₂S₄]^4–). The reaction with white phosphorus (P₄) generates an unusual Ar’P₄Sn₂Ar’ ligand. This multifaceted reactivity illustrates the behavior of the Fe and Sn sites in complex <b>1</b>, suggesting that complexes of this type are promising reagents for small molecule activation.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"21 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Charge Density Wave and Superconductivity in BaSbTe2S Heterolayer Crystal with 2D Te Square Nets","authors":"Zhong-Zhen Luo, Hengdi Zhao, Weizhao Cai, Shima Shahabfar, Juncen Li, Songting Cai, Jameson Berg, Tushar Bhowmick, Jin-Ke Bao, Shiqiang Hao, Yihui He, Weiping Guo, Duck Young Chung, Yan Yu, Suchismita Sarker, Matthew Grayson, Christopher Wolverton, Vinayak P. Dravid, Wendan Cheng, Zhigang Zou, Stephan Rosenkranz, Christos D. Malliakas, Shanti Deemyad, Mercouri G. Kanatzidis","doi":"10.1021/jacs.4c16505","DOIUrl":"https://doi.org/10.1021/jacs.4c16505","url":null,"abstract":"Low-dimensional materials with charge density waves (CDW) are attractive for their potential to exhibit superconductivity and nontrivial topological electronic features. Here we report the two-dimensional (2D) chalcogenide, BaSbTe₂S which acts as a new platform hosting these phenomena. The crystal structure of BaSbTe₂S is composed of alternating atomically thin Te square-net layers and double rock-salt type [(SbTeS)₂]^2– slabs separated with Ba²⁺ atoms. Due to the electronic instability of the Te square net, an incommensurately modulated structure is triggered and confirmed by both single-crystal X-ray diffraction, electron diffraction, and the presence of an energy bandgap in this compound. Our first-principles electronic structure analysis and investigation of structural dynamical instability suggest that the Te network plays a dominant role in its origin. The incommensurate structure is refined with a modulation vector of <i><b>q</b></i> = 0.351(1)<i>b</i>* using an orthorhombic cell of <i>a</i> = 4.4696(5) Å, <i>b</i> = 4.4680(5) Å, and <i>c</i> = 15.999(2) Å under superspace group <i>Pmm</i>2(0β0)000 at 293 K. The modulation vector <i><b>q</b></i> varies as a function of both occupancy of Te in the square net and temperature, indicating the CDW order can be modulated by local distortions. The CDW can be suppressed by pressure, leading to the emergence of superconductivity with a <i>T</i>_c up to 7.5 K at 13.6 GPa, suggesting a competition between the CDW order and superconductivity. Furthermore, electrical transport under the magnetic field reveals the existence of compensated high mobility electron- and hole-bands near the Fermi surface (μ ∼600–3500 cm²V^–1s^–1), suggesting Dirac-like band dispersion.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"65 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Host–Guest Chemistry-Mediated Biomimetic Chemoenzymatic Synthesis of Complex Glycosphingolipids","authors":"Yuan Ma, Yating Liu, Chang Cao, Jiarong Peng, Yinyu Jiang, Tiehai Li","doi":"10.1021/jacs.4c17725","DOIUrl":"https://doi.org/10.1021/jacs.4c17725","url":null,"abstract":"Glycosphingolipids (GSLs) are amphipathic complex biomolecules constituted of hydrophilic glycans covalently linked to hydrophobic lipids via glycosidic bonds. GSLs are widely distributed in cells and tissues, where they play crucial roles in various biological functions and disease processes. However, the heterogeneity and complexity of GSLs make it difficult to explore their precise biofunctions due to obstacles in obtaining well-defined structures. Herein, we report a host–guest-chemistry-mediated biomimetic chemoenzymatic approach for the efficient synthesis of diverse complex GSLs. A key feature of this approach is that the use of methyl-β-cyclodextrin enables amphipathic glycolipids forming water-soluble inclusion complexes to improve their solubility in aqueous media, thereby facilitating enzyme-catalyzed reactions. The power and applicability of our approach are demonstrated by the streamlined synthesis of biologically important globo-, ganglio-, neolacto-, and lacto-series GSLs library containing 20 neutral and acidic glycolipids with different fucosylation and sialylation patterns. The developed method will open new avenues to easily access a wide range of complex GSLs for biomedical applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"86 2 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Reduction-Interrupted Tandem Reaction for General Synthesis of Functional Amino Acids by a Heterogeneous Cobalt Catalyst","authors":"Haotian Hua, Chenggang Ci, Pierre H. Dixneuf, Min Zhang","doi":"10.1021/jacs.4c15284","DOIUrl":"https://doi.org/10.1021/jacs.4c15284","url":null,"abstract":"Despite their significant importance in numerous fields, the challenges in direct and diverse synthesis of γ-amino-α-hydroxybutyric acids (AHBAs) pose substantial obstacles to explore their functions. Here, by preparation of a <i>N</i>-doped carbon-supported bifunctional cobalt catalyst (Co-DAPhen/C), it was applied to develop a reductive tandem reaction for general synthesis of AHBA derivatives from cheap and abundant nitroarenes, formaldehyde, and acrylates. This catalytic three-component reaction features broad substrate and functionality tolerance, an easily accessible and reusable catalyst, and high step and atom economy. The active Co sites of the catalyst are involved in the mild reduction processes with formic acid, whereas the N-doped carbon support enriches the HCHO and acrylates by physical adsorption, thus favoring the capture of hydroxylamine and nitrone intermediates via condensation and 1,3-dipolar cycloaddition, respectively. Such a metal–support synergy interrupts the conventional reduction of nitroarenes into anilines and results in a novel tandem reaction route. In this work, the concept merging mild reduction and effective intermediate transformations is anticipated to develop more useful tandem reactions by rational catalyst design.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"41 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393865","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Molecular Self-Gating Inside a Zeolite Catalyst","authors":"Zhiqiang Liu, Caiyi Lou, Jiamin Yuan, Xiaomin Tang, Yuzhou Fan, Ji Qi, Rui Zhang, Peng Peng, Guoliang Liu, Shutao Xu, Anmin Zheng","doi":"10.1021/jacs.4c17510","DOIUrl":"https://doi.org/10.1021/jacs.4c17510","url":null,"abstract":"Diffusion is a ubiquitous process that is strongly correlated with concentration. Based on developed three-dimensional free energy and a continuous-time random-walk coarse-graining method, we found the optimal diffusion pathway under confinement, determined all diffusional energy barriers, and identified the major units of zeolite where molecular diffusion is limited. Interestingly, a novel diffusion mechanism was determined in the nanopore of a zeolite catalyst by molecular dynamics simulation, pulsed field gradient, and 2D exchange spectroscopy (EXSY) NMR experiments. We describe a “molecular self-gating effect” that effectively predominates the diffusion process in cage-type (e.g., RHO and MER) zeolites through a “traffic jam” and a “smooth traffic” process. Initially, transport is hindered by molecules forming a gate (traffic jam); then, as the number of molecules reaches a certain threshold, diffusion increases rapidly due to the synergistic collisions of aggregated molecules upon the gate (smooth traffic). This unique diffusion behavior is observed here for the first time and illustrates a microscopic mechanism dictated by the molecular self-gating effect in a confined space. The exploitable diffusion disclosed herein should shed new light on the fundamental understanding of transport, as well as enrich diffusion behavior under confinement.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"13 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385035","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}