ACS Catalysis 最新文献

{"title":"Insights into the Surface Electronic Structure and Catalytic Activity of InOx/Au(111) Inverse Catalysts for CO2 Hydrogenation to Methanol","authors":"Kasala Prabhakar Reddy, Yi Tian, Pedro J. Ramírez, Arephin Islam, Hojoon Lim, Ning Rui, Yilin Xie, Adrian Hunt, Iradwikanari Waluyo, José A. Rodriguez","doi":"10.1021/acscatal.4c05837","DOIUrl":"https://doi.org/10.1021/acscatal.4c05837","url":null,"abstract":"The direct conversion of carbon dioxide (CO₂) into methanol (CH₃OH) via low-temperature hydrogenation is crucial for recycling anthropogenic CO₂ emissions and producing fuels or high value chemicals. Nevertheless, it continues to be a great challenge due to the trade-off between selectivity and catalytic activity. For CO₂ hydrogenation, In₂O₃ catalysts are known for their high CH₃OH selectivity. Subsequent studies explored depositing metals on In₂O₃ to enhance CO₂ conversion. Despite extensive research on metal (M) supported In₂O₃ catalysts, the role of In–M alloys and M/In₂O₃ interfaces in CO₂ activation and CH₃OH selectivity remains unclear. In this work, we have examined the behavior of In/Au(111) alloys and InO_<i>x</i>/Au(111) inverse systems during CO₂ hydrogenation using synchrotron-based ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) and catalytic tests in a batch reactor. Indium forms alloys with Au(111) after deposition. The In–Au(111) alloys display high reactivity toward CO₂ and can dissociate the molecule at room temperature to generate InO_<i>x</i> nanostructures. At very low coverages of In (≤0.05 ML), the InO_<i>x</i> nanostructures are not stable under CO₂ hydrogenation conditions and the active In–Au(111) alloys produces mainly CO and little methanol. An increase in indium coverage to 0.3 ML led to stable InO_<i>x</i> nanostructures under CO₂ hydrogenation conditions. These InO_<i>x</i>/Au(111) catalysts displayed a high selectivity (∼80%) toward CH₃OH production and an activity for CO₂ conversion that was at least 10 times larger than that of plain In₂O₃ or Cu(111) and Cu/ZnO(0001̅) benchmark catalysts. The results of AP-XPS show that InO_<i>x</i>/Au(111) produces methanol via methoxy intermediates. Inverse oxide/metal catalysts containing InO_<i>x</i> open up a possibility for improving CO₂ → CH₃OH conversion in processes associated with the control of environmental pollution and the production of high value chemicals.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588984","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":"Substrate-Dependent Role of a Pd Dopant in PdAu12 Catalysts in the Oxidation of p-Substituted Benzyl Alcohols: Promotion of Hydride Abstraction and Reductive Activation of O2","authors":"Shinya Masuda, Haru Hirai, Pei Zhao, Shinjiro Takano, Masahiro Ehara, Tatsuya Tsukuda","doi":"10.1021/acscatal.4c03871","DOIUrl":"https://doi.org/10.1021/acscatal.4c03871","url":null,"abstract":"Single-atom doping, which is the primary step toward multimetallization, on atomically size-controlled metal nanoclusters facilitates the elucidation of doping effects on catalysis. Herein, we synthesized MAu₁₂ (M = Au, Ir, Rh, Pt, or Pd) nanoclusters on double metal hydroxide composed of Co and Ce by thermal treatment of diphosphine-protected MAu₁₂(dppe)₅Cl₂ (dppe: 1,2-bis(diphenylphosphino)ethane). The successful formation of the MAu₁₂ nanocluster under an optimized thermal treatment condition (175 °C, 8 h) was confirmed by X-ray absorption fine structure spectroscopy and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy. Among the five catalysts, PdAu₁₂ exhibited 4.4 times higher activity than Au₁₃ in the aqueous phase benzyl alcohol (BnOH) oxidation, while the other MAu₁₂ (M = Ir, Rh, or Pt) catalysts showed comparable activity to Au₁₃. On the basis of the kinetic experiments under different partial pressures of O₂ with <i>p</i>-substituted BnOH (R-BnOH; R = MeO, Me, H, Cl, or CF₃), we concluded that the single Pd atom dopant plays a dual role in the oxidation depending on the nature of the R group: abstraction of H^– from the adsorbed alkoxide for R = Cl or CF₃ and reductive activation of O₂ for R = MeO, Me, or H. Theoretical studies on model structures have shown that O₂ is more efficiently activated by PdAu₁₂ than by Au₁₃, thereby the different mechanism mediated by activated O₂ appears with the single Pd doping.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589018","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":"Fluorescence Lifetime Imaging Microscopy (FLIM) as a Tool to Understand Chemical Reactions and Catalysis","authors":"Pía A. López, Suzanne A. Blum","doi":"10.1021/acscatal.4c05450","DOIUrl":"https://doi.org/10.1021/acscatal.4c05450","url":null,"abstract":"Fluorescence lifetime imaging microscopy (FLIM) is an emerging tool to characterize ongoing chemical reactions in synthetic chemistry and catalysis. Initially applied to biological systems, FLIM now reveals spatially resolved chemical reaction species and system-wide physiochemical changes that accompany ongoing reactions. FLIM combines the advantage of environmental sensitivity with high signal sensitivity (as sensitive as single molecules) and has the key ability to operate under synthetic conditions (e.g., high concentrations of reagents, in organic solvents, under ambient temperature and pressure, in opaque mixtures, and in multiphasic systems). Chemical reactions inherently induce changes in the reaction medium, neighboring compounds, surface compositions, and/or bonding structure of the compounds involved, resulting in environmental changes. The FLIM methods recently developed harness and interpret these changes in ways that lead to characterizing compounds and enhancing a mechanistic understanding. Here, current advantages and limitations of FLIM methods are considered, common factors influencing fluorescence lifetime in chemical systems are discussed in a tutorial format, and seven research case studies are strategically analyzed, chosen to highlight how FLIM provided complementary information to understand chemical reaction mechanisms, intermediates, product distributions, partitioning, roles of reagents, and catalyst behaviors. These data and insights obtained from FLIM assist in the rational design and optimization of synthetic and catalytic methods.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589020","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":"Operando Scanning Electrochemical Microscopy Reveals Facet-Dependent Structure–Selectivity Relationship for CO2 Reduction on Gold Surfaces","authors":"Yunwoo Nam, Sung-Eun Cho, Hyun S. Ahn","doi":"10.1021/acscatal.4c05007","DOIUrl":"https://doi.org/10.1021/acscatal.4c05007","url":null,"abstract":"Selective and efficient electrochemical conversion of CO₂ to useful chemical feedstocks requires a comprehensive understanding of the reaction mechanism and revelation of the key structural characteristics of good catalysts via in situ and <i>operando</i> surface analyses of the working electrode. To achieve this, an electrochemical method was developed on the scanning electrochemical microscopy (SECM) platform. The electrochemical surface analysis is termed sequential voltammetric SECM (SV-SECM), which allows for simultaneous detection of various CO₂ reduction reaction products. Operando mapping of the activity was carried out on gold surfaces to reveal distinct facet-dependent product selectivity when overlaid with crystal orientation maps. Notably, we verified that crystal grains rich in (111) surfaces demonstrate superior CO₂ reduction selectivity compared to that with (100) surfaces. The analytical platform developed here was implemented on electrochemical reduction of CO₂ on gold as a proof-of-concept; however, it should be readily expandable to reactions yielding complex product selectivity distribution with an ill-understood catalytic structure–activity relationship.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588386","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":"Valence Electron and Coordination Structure Guided Metal Active Site Design for Hydrolytic Cleavage of Carbon–Sulfide Double Bonds","authors":"Ganchang Lei, Xiaoyun Lin, Hongping Yan, Lijuan Shen, Shiping Wang, Shijing Liang, Zhi-Jian Zhao, Fujian Liu, Yingying Zhan, Lilong Jiang","doi":"10.1021/acscatal.4c02921","DOIUrl":"https://doi.org/10.1021/acscatal.4c02921","url":null,"abstract":"The catalytic cleavage of carbon–sulfur (C═S) double bonds on the metal sites without deactivation has aroused great interest in both fundamental catalytic research and industrial chemistry. Herein, activity descriptors are developed via machine learning and density functional theory (DFT) calculations to screen transition-metal single-site catalysts, which quantify the effect of both atomic electronic properties and coordination configuration on the hydrolysis of C═S double bonds. The valence electron number and electronegativity of active sites are found to be well related to C═S activation and sulfur poisoning, where Fe demonstrates high catalytic potential among a series of metal centers. On the other hand, the isolated Fe₁ and Fe₂ sites favor carbonyl sulfide (COS) adsorption and activation, while the COS easily dissociates into *S and *CO on Fe₃ hollow site, thus resulting in the formation of robust Fe–S bonds and catalyst deactivation. As anticipated, the as-designed Fe₁–N₄ site achieves a COS conversion of ca. 96% at 100 °C, slightly better than the Fe₂–N₄ site, approximately 8 times higher than that of the Fe/C, which is also better than those of other monatomic catalysts (such as Co-NC, Ni-NC, Sn-NC, and Bi-NC). The combination of in situ characterizations and theoretical calculations suggests that *COS and *H₂O/*OH have a competitive adsorption relationship on Fe–N₄ sites, and two Fe–N₄ sites can synergistically catalyze the COS hydrolysis through the spilled H and OH.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588385","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":"Nitrite-Mediated Pulsed Electrocatalytic Nitrate Reduction to Ammonia over Co@Cu NW with Dual Active Sites","authors":"Rundong Zhao, Qiuyu Yan, Ling Lu, Lihong Yu, Huang Chen, Tian Yan, Le Liu, Jingyu Xi","doi":"10.1021/acscatal.4c03782","DOIUrl":"https://doi.org/10.1021/acscatal.4c03782","url":null,"abstract":"As a potential alternative to the Haber–Bosch process for ammonia (NH₃) synthesis, the electrocatalytic nitrate reduction reaction (NO₃RR) has attracted extensive attention. The electrocatalytic conversion of NO₃^– to NH₃ involves a complex 8e^– reaction with various byproducts. By decomposing the overall reaction into a 2e^– process from NO₃^– to NO₂^– and a 6e^– process from NO₂^– to NH₃, the two-step reaction can be strategically optimized to achieve efficient tandem catalysis. This work developed a NO₂^–-mediated pulsed electrocatalytic NO₃RR by Co@Cu nanowire (NW) with dual active sites of the Co phase and Cu phase. The Cu phase rapidly accumulates NO₂^– at low potentials, while the Co phase efficiently converts NO₂^– to NH₃ at high potentials, completing a time-separated tandem catalytic reaction. Ultimately, the Co@Cu NW achieved a maximum NH₃ yield rate of 5148.6 μg·h^–1·cm^–2 and a maximum Faraday efficiency of 88.6% under pulsed potentials of −0.2 and −0.7 V versus the reversible hydrogen electrode in an electrolyte of 0.5 M SO₄^2– and 0.1 M NO₃^–. Furthermore, <i>in situ</i> reflection absorption imaging and <i>in situ</i> total internal reflection imaging revealed that the pulsed strategy effectively enhances the utilization of NO₂^– and suppresses competitive hydrogen evolution reaction, thereby improving NO₃RR performance.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580545","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":"Keeping the Distance: Activity Control in Solid-Supported Sucrose Phosphorylase by a Rigid α-Helical Linker of Tunable Spacer Length","authors":"Chao Zhong, Anisha Vyas, Jakob D. H. Liu, Chris Oostenbrink, Bernd Nidetzky","doi":"10.1021/acscatal.4c05616","DOIUrl":"https://doi.org/10.1021/acscatal.4c05616","url":null,"abstract":"Enzyme immobilization into carrier materials has broad importance in biotechnology, yet understanding the catalysis of enzymes bound to solid surfaces remains challenging. Here, we explore surface effects on the catalysis of sucrose phosphorylase through a fusion protein approach. We immobilize the enzyme via a structurally rigid α-helical linker [EA₃K]_<i>n</i> of tunable spacer length due to the variable number of pentapeptide repeats used (<i>n</i> = 6, 14, 19). Molecular modeling and simulation approaches delineate the conformational space sampled by each linker relative to its His-tag cap used for surface tethering. The population distribution of linker conformers gets broader, with a consequent shift of the enzyme-to-surface distance to larger values (≤15 nm), as the spacer length increases. Based on temperature kinetic studies, we obtain an energetic description of catalysis by the enzyme-to-linker fusions in solution and immobilize on Ni²⁺-chelate agarose. The solid-supported enzymes involve distinct changes in enthalpy–entropy partitioning within the frame of invariant Gibbs free energy of activation (Δ<i>G</i>^‡ = ∼61 kJ/mol at 30 °C). The entropic contribution (−<i>T</i>Δ<i>S</i>^‡) to Δ<i>G</i>^‡ increases with the spacer length, from −16.4 kJ/mol in the linker-free enzyme to +7.9 kJ/mol in the [EA₃K]₁₉ linked fusion. The immobilized [EA₃K]₁₉ fusion protein is indistinguishable in its catalytic properties from the enzymes in solution, which behave identically regardless of their linker. Enzymes positioned closer to the surface arguably experience a higher degree of molecular organization (“rigidification”) that must relax for catalysis through the additional uptake of heat, compensated by a gain in entropy. Increased thermostability of these enzymes (up to 2.8-fold) is consistent with the proposed rigidification effect. Collectively, our study reveals surface effects on the activation parameters of sucrose phosphorylase catalysis and shows their consistent dependence on the length of the surface-tethering linker. The fundamental insight here obtained, together with the successful extension of the principle to a different enzyme (nigerose phosphorylase), suggests that rigid linker-based control of the protein–surface distance can be used as an engineering strategy to optimize the activity characteristics of immobilized enzymes.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588388","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":"Enabling Site-Selective C–H Functionalization of Aliphatic Alcohols and Amines with exo-Directing Groups by Tether-Tunable Design of PdII/PdIV Catalysis","authors":"Kang Fu, Lei Shi","doi":"10.1021/acscatal.4c05553","DOIUrl":"https://doi.org/10.1021/acscatal.4c05553","url":null,"abstract":"We report herein a general platform for palladium catalysis using a library of cyclic diacyl peroxides, achieving site-selective C–H functionalization of aliphatic alcohols and amines. Experimental studies and theoretical calculations indicate that bystanding cyclic diacyl peroxides minimize unwanted reductive elimination events and enable controlled C–H cleavage. The protocol is simple and scalable and offers high selectivity and a broad range of substrates and nucleophiles, including complex molecules. The findings advance understanding of high-valent palladium chemistry, providing a tool for creating chemically diverse vicinal diols and amino alcohols and opening new possibilities in C–H functionalization.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588387","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":"Manganese–Palladium Dual-Atom Catalyst Boosts Direct H2O2 Synthesis beyond 2 wt % at Atmospheric Conditions","authors":"Guancong Jiang, Lihui Mou, Zhiheng Wang, Lilong Zhang, Tuo Ji, Liwen Mu, Jun Jiang, Xiaohua Lu, Jiahua Zhu","doi":"10.1021/acscatal.4c04446","DOIUrl":"https://doi.org/10.1021/acscatal.4c04446","url":null,"abstract":"Direct synthesis of hydrogen peroxide (H₂O₂) from H₂ and O₂ is appealing due to its nonpolluting nature, yet it is still very challenging to meet both high productivity and selectivity. In this work, a simple strategy was developed to synthesize a highly efficient dual-atom catalyst with a Mn atom inherited from nature biomass and a Pd atom artificially synthesized, which boosts a very high H₂O₂ productivity of 46,798 mmol g_Pd^–1 h^–1 and high selectivity of 89% even under atmospheric conditions (1 atm, 25 °C). Such high-efficiency catalysis enabled the production of a H₂O₂ solution with concentration beyond 2 wt %, which has not been achieved in earlier work. Experimental characterizations revealed the great H₂ dissociation capability on the Pd–Mn/SMC (SMC = sylvestris mesoporous carbon) catalyst that was responsible for the high productivity. Theoretical calculations confirmed the favorable hydrogenation of undissociated O₂ to H₂O₂ on the Pd–Mn dual-atom structure, which thus achieved high selectivity. Overall, this work provides a simple perspective on the utilization of natural species in biomass for single-atom structure fabrication and catalyst development for emerging applications.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589054","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":"Systematic Parameter Determination Aimed at a Catalyst-Controlled Asymmetric Rh(I)-Catalyzed Pauson–Khand Reaction","authors":"Yifan Qi, Luke T. Jesikiewicz, Grace E. Scofield, Peng Liu, Kay M. Brummond","doi":"10.1021/acscatal.4c04490","DOIUrl":"https://doi.org/10.1021/acscatal.4c04490","url":null,"abstract":"Transition metal-catalyzed carbocyclization reactions have revolutionized the synthesis of complex cyclic organic compounds. Yet, subtle substrate changes can significantly alter reaction pathways. The asymmetric Rh(I)-catalyzed Pauson<b>–</b>Khand reaction (PKR) exemplifies such a reaction, hindered by a narrow substrate scope and competing reactivity modes. In this study, we identified parameters predictive of the yield and enantioselectivity in the catalyst-controlled asymmetric PKR, using 1,6-enynes with a 2,2-disubstituted alkene. In this way, ring-fused cyclopentenones can be formed with chiral quaternary carbon centers. Using bisphosphine ligand parameters from palladium complexes, including the energy of the Pd lone pair orbital and the angle formed by the phosphorus aryl groups on the ligand, we established strong correlations with experimental ln(<i>er</i>) (<i>R</i>² = 0.99 and 0.91) for two distinct precursors. Solvent dipole moments correlated with ln(<i>er</i>) for high-dipole-moment precursors (<i>R</i>² = 0.94), while Abraham’s hydrogen bond basicity is more relevant for low-dipole-moment precursors (<i>R</i>² = 0.93). Additionally, counterions were found to have a significant impact on the PKR reactivity and selectivity, as does the steric demand of the alkyne substituent of the enyne precursor. In the latter case, ln(<i>er</i>) correlates with Sterimol B₁ values for products from different alkyne substituents (<i>R</i>² = 0.99). Furthermore, the computed C≡C wavenumber of the enyne precursor can be directly aligned with the yield of asymmetric PKRs.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":12.9,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588985","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}