Li‐Xue Jiang

Purdue University West Lafayette

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Sheng‐Gui He

Chinese Academy of Sciences

Xiao‐Na Li

Beijing Institute of Technology

Yan‐Xia Zhao

Beijing National Laboratory for Molecular Sciences

Qing‐Yu Liu

Chinese Academy of Sciences

Qiang Chen

Shanxi University

Haifang Li

North China Electric Power University

Julia Laskin

Purdue University West Lafayette

Jiaojiao Chen

Shenyang University of Chemical Technology

Lina Wang

Sun Yat-sen University

Yi Ren

National University of Defense Technology

Cooperative Institutions

Chinese Academy of Sciences

Beijing National Laboratory for Molecular Sciences

Institute of Chemistry

University of Chinese Academy of Sciences

Purdue University West Lafayette

Jilin University

State Key Laboratory for Structural Chemistry of Unstable and Stable Species

Sun Yat-sen University

South China University of Technology

Beijing Institute of Technology

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Catalytic CO Oxidation by O₂ Mediated by Noble‐Metal‐Free Cluster Anions Cu₂VO_3–5⁻

Angewandte Chemie International Edition (2018)

Lina Wang Xiao‐Na Li Li‐Xue Jiang Bin Yang Qing‐Yu Liu

Abstract Catalytic CO oxidation by molecular O 2 is an important model reaction in both the condensed phase and gas‐phase studies. Available gas‐phase studies indicate that noble metal is indispensable in catalytic CO oxidation by O 2 under thermal collision conditions. Herein, we identified the first example of noble‐metal‐free heteronuclear oxide cluster catalysts, the copper–vanadium bimetallic oxide clusters Cu 2 VO 3–5 − for CO oxidation by O 2 . The reactions were characterized by mass spectrometry, photoelectron spectroscopy, and density functional calculations. The dynamic nature of the Cu−Cu unit in terms of the electron storage and release is the driving force to promote CO oxidation and O 2 activation during the catalysis.

Bimetallic strip

Heteronuclear molecule

Vanadium Oxide

Noble metal

10.1002/anie.201712129

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Citations (48)

Mechanistic Variants in Methane Activation Mediated by Gold(I) Supported on Silicon Oxide Clusters

Chemistry - A European Journal (2018)

Yi‐Ming Chen Lina Wang Jiao‐Jiao Chen Qiang Chen Li‐Xue Jiang

Abstract Cationic gold has been frequently identified as a suitable reactive species for activating methane in condensed‐phase studies. However, it is far from clear how the coordination site manipulates the activity of such species. Herein, by anchoring Au I on silicon oxide cluster supports of variable sizes, the site‐specific methane activation by Au I −O x has been clarified by mass spectrometry in conjunction with quantum chemistry calculations. An unexpected mechanistic switch in C−H activation was identified for the cluster anions Au(SiO 2 ) n O − ( n= 1–3) that selectively activate one of the four C−H bonds of methane with different reaction efficiencies: a low efficiency was observed for the two‐fold‐coordinated gold ion (Au I, 2f ), which was anchored on an AuSiO 3 − or AuSi 2 O 5 − cluster, through an oxidative addition mechanism (a homolytic process), and high efficiency was observed for the one‐fold‐coordinated gold ion (Au I, 1f ), which was supported on an AuSi 3 O 7 − cluster, through Lewis acid/base pairs mechanism (Au I, 1f ⋅⋅⋅O 2− , a heterolytic process). Fine regulation of the 5d orbital level of the Au atom by the oxygen ligands accounted for the mechanistic difference between Au I, 2f and Au I, 1f species. The mechanistic understanding of the reactivity of Au I −O x at a strictly molecular level can be used to clarify the dissimilar activity of gold anchored on different oxide supports.

Heterolysis

Homolysis

Reactivity

Cationic polymerization

10.1002/chem.201803432

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Citations (7)

Electron Attachment Reaction Ionization of Gas-Phase Methylglyoxal

Analytical Chemistry (2018)

Xue-wei Lü Yi Ren Qing‐Yu Liu Ting Zhang Li‐Xue Jiang

Methylglyoxal (MGLY) plays a significant role in atmospheric chemistry by serving as a key contributor to the formation of active free radicals, ozone, and secondary organic aerosol. Detection of MGLY by traditional chemical ionization such as proton-transfer reaction has several shortcomings such as parent molecule fragmentation. In this study, an electron attachment reaction (EAR) ionization method has been developed for the effective detection of MGLY. Almost no fragmentation was observed during the EAR. The generation of MGLY- anion in the EAR was further confirmed by cryogenic photoelectron imaging spectroscopy. The concentration of MGLY can be calibrated by using dibromomethane (CH2Br2) as reference gas. The detection sensitivity of MGLY was estimated to be (100 ± 2) mV/ppbv (parts per billion by volume). The O2, H2O, CO2, and trace gases in ambient air have no obvious effects on the detection of MGLY- anion by the EAR ionization method.

10.1021/acs.analchem.8b03305

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Citations (3)

Catalytic CO Oxidation by O₂ Mediated by Noble‐Metal‐Free Cluster Anions Cu₂VO_3–5⁻

Angewandte Chemie (2018)

Lina Wang Xiao‐Na Li Li‐Xue Jiang Bin Yang Qing‐Yu Liu

Bimetallic strip

Heteronuclear molecule

Noble metal

Vanadium Oxide

10.1002/ange.201712129

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Citations (13)

An Eight-Atom Iridium–Aluminum Oxide Cluster IrAlO₆⁺ Catalytically Oxidizes Six CO Molecules

The Journal of Physical Chemistry Letters (2019)

Xiao‐Na Li Li‐Xue Jiang Lina Wang Shu-Hua Ou Meiqi Zhang

Fundamental understanding regarding oxygen storage capacity involving how and why an active site can buffer a large number of oxygen atoms in redox processes is vital to the design of advanced oxygen storage materials, while it is challenging because of the complexity of heterogeneous catalysis. Herein, we identified that an eight-atom iridium-aluminum oxide cluster IrAlO6+ can transfer all the oxygen atoms to catalytically oxidize six CO molecules. This finding represents a breakthrough in cluster catalysis where at most three oxygen atoms from a heteronuclear metal oxide cluster can be catalytically involved in CO oxidation. We found that oxygen prefers to be stored on aluminum to form an O3-• radical in the energetically unfavorable IrAlO6+ isomer and generate the low-coordinated iridium that is pivotal to capturing CO and triggering the catalysis. The powerful electron cycling capability of iridium and the cooperative iridium-aluminum interplay are emphasized to drive the oxygen atom-transfer behavior.

Aluminum Oxide

10.1021/acs.jpclett.9b03056

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Neutral Au₁-Doped Cluster Catalysts AuTi₂O_3–6 for CO Oxidation by O₂

Journal of the American Chemical Society (2018)

Jiaojiao Chen Xiao‐Na Li Qiang Chen Qing‐Yu Liu Li‐Xue Jiang

Oxide supported gold catalysts (e.g., Au/TiO2) are of great significance in heterogeneous catalysis owing to their extraordinary catalytic activity. Study of heteronuclear metal oxide clusters (HMOCs, e.g., AuxTiyOzq) is an important way to uncover the molecular-level mechanisms of gold catalysis in the related heterogeneous catalytic systems. However, the current studies of HMOCs are focused on charged clusters with little attention paid to neutral species. The reactivity study of neutral HMOCs is vital to have a comprehensive understanding of heterogeneous catalysis, but it is experimentally challenging because of the difficulty of cluster ionization and detection without fragmentation. Herein, benefiting from a homemade time-of-flight mass spectrometer coupled with a vacuum ultraviolet laser system, the reactivity of neutral Au1-doped titanium oxide clusters AuTi2O3–6 in catalytic CO oxidation by O2 has been successfully identified. The mechanistic details of the catalysis have been elucidated by quantum chemistry calculations. The crucial roles of the mobile AuCO species that can facilitate not only the process of CO oxidation but also the process of O2 activation have been discovered in the cluster catalysis. The fascinating results are of substantial importance to understand the mechanisms of CO oxidation over Au/TiO2, one type of the best studied gold catalysts.

Heteronuclear molecule

Reactivity

Titanium oxide

Catalytic cycle

10.1021/jacs.8b11118

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Formaldehyde Generation in Photooxidation of Isoprene on Iron Oxide Nanoclusters

The Journal of Physical Chemistry C (2019)

Shi-Ying Lv Qing‐Yu Liu Yan‐Xia Zhao Meiqi Zhang Li‐Xue Jiang

The photooxidation of isoprene (C5H8) dominates the source of formaldehyde (CH2O) in the atmosphere. The isoprene degradation initiated by atmospheric radicals has been well understood. However, the potential role of metal-oxide particles, which are important components of mineral dust, has not been well studied. Herein, the generation of CH2O through photooxidation of isoprene on iron oxide clusters (FexOy+, 3 ≤ x ≤ 23, 3 ≤ y ≤ 35) up to a nanosize has been identified successfully by mass spectrometric experiments. Theoretical studies indicate that the production of CH2O from the C5H8 adsorption complex has to overcome a significant barrier and the photo-irradiation can accelerate this process. The product selectivity of CH2O can be enhanced by visible light irradiation with respect to ultraviolet irradiation. The large-sized clusters can be more efficient to generate CH2O in a gas-particle interaction system. This study can provide a new source of formaldehyde from the photooxidation of isoprene on iron oxide-based mineral dust in the atmosphere.

Isoprene

Nanoclusters

Ultraviolet

10.1021/acs.jpcc.8b12471

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Citations (9)

Direct Conversion of Methane with Carbon Dioxide Mediated by RhVO₃⁻ Cluster Anions

Angewandte Chemie (2019)

Yuan Yang Bin Yang Yan‐Xia Zhao Li‐Xue Jiang Ziyu Li

Abstract Direct conversion of methane with carbon dioxide to value‐added chemicals is attractive but extremely challenging because of the thermodynamic stability and kinetic inertness of both molecules. Herein, the first dinuclear cluster species, RhVO 3 − , has been designed to mediate the co‐conversion of CH 4 and CO 2 to oxygenated products, CH 3 OH and CH 2 O, in the temperature range of 393–600 K. The resulting cluster ions RhVO 3 CO − after CH 3 OH formation can further desorb the [CO] unit to regenerate the RhVO 3 − cluster, leading to the successful establishment of a catalytic cycle for methanol production from CH 4 and CO 2 (CH 4 +CO 2 →CH 3 OH+CO). The exceptional activity of Rh‐V dinuclear oxide cluster (RhVO 3 − ) identified herein provides a new mechanism for co‐conversion of two very stable molecules CH 4 and CO 2 .

Carbon fibers

10.1002/ange.201911195

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Citations (14)

Nanospray desorption electrospray ionization (nano-DESI) mass spectrometry imaging with high ion mobility resolution

Li‐Xue Jiang Emerson L. Hernly Hang Hu Ryan T. Hilger Heiko Neuweger

Untargeted separation of isomeric and isobaric species in mass spectrometry imaging (MSI) is challenging. The combination of ion mobility spectrometry (IMS) with MSI has emerged as an effective strategy for differentiating isomeric and isobaric species, which substantially enhances the molecular coverage and specificity of MSI experiments. In this study, we have implemented nanospray desorption electrospray ionization (nano-DESI) MSI on a trapped ion mobility spectrometry (TIMS) mass spectrometer. A new nano-DESI source was constructed, and a specially designed inlet extension was fabricated to accommodate the new source. The nano-DESI-TIMS-MSI platform was evaluated by imaging mouse brain tissue sections. We achieved high ion mobility resolution by utilizing three narrow mobility scan windows that cover the majority of the lipid molecules. Notably, the mobility resolution reaching up to 300 in this study is much higher than the resolution obtained in our previous study using drift tube IMS. High-resolution TIMS successfully separated lipid isomers and isobars revealing their distinct localizations in tissue samples. Our results further demonstrate the power of high mobility resolution IMS for unraveling the complexity of biomolecular mixtures analyzed in MSI experiments.

Ion-mobility spectrometry

Desorption electrospray ionization

Mass spectrometry imaging

Isobar

MALDI imaging

10.26434/chemrxiv-2023-73g9n

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Citations (1)

Nanospray Desorption Electrospray Ionization (Nano-DESI) Mass Spectrometry Imaging with High Ion Mobility Resolution

Journal of the American Society for Mass Spectrometry (2023)

Li‐Xue Jiang Emerson Hernly Hang Hu Ryan T. Hilger Heiko Neuweger

Untargeted separation of isomeric and isobaric species in mass spectrometry imaging (MSI) is challenging. The combination of ion mobility spectrometry (IMS) with MSI has emerged as an effective strategy for differentiating isomeric and isobaric species, which substantially enhances the molecular coverage and specificity of MSI experiments. In this study, we have implemented nanospray desorption electrospray ionization (nano-DESI) MSI on a trapped ion mobility spectrometry (TIMS) mass spectrometer. A new nano-DESI source was constructed, and a specially designed inlet extension was fabricated to accommodate the new source. The nano-DESI-TIMS-MSI platform was evaluated by imaging mouse brain tissue sections. We achieved high ion mobility resolution by utilizing three narrow mobility scan windows that covered the majority of the lipid molecules. Notably, the mobility resolution reaching up to 300 in this study is much higher than the resolution obtained in our previous study using drift tube IMS. High-resolution TIMS successfully separated lipid isomers and isobars, revealing their distinct localizations in tissue samples. Our results further demonstrate the power of high-mobility-resolution IMS for unraveling the complexity of biomolecular mixtures analyzed in MSI experiments.

Ion-mobility spectrometry

Desorption electrospray ionization

Mass spectrometry imaging

Isobar

MALDI imaging

Isobaric process

10.1021/jasms.3c00199

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Citations (23)