RAPID COMMUNICATIONS IN MASS SPECTROMETRY
·
2021
·Vol. 36
·期 3
·e9218
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IF 2.419
Mengying Du,Kailin Zhang,Luyang Jiao,Yicheng Xu,Xianglei Kong
Rationale The challenge of glycan identification due to their structural complexity and diversity has profited enormously from recent developments in mass spectrometry (MS)-related methods. For photodissociation MS, infrared (IR) and ultraviolet (UV) lasers can generate complementary fragment ions, so an effective combination of the two methods may provide rich and valuable fragmentation patterns for glycan analysis. Methods A 7.0 T Fourier transform ion cyclotron resonance (FTICR) mass spectrometer equipped with a double-beam laser system was applied for the experiments. 3,5-Diiodo-L-tyrosine was selected as the assistant molecule to form complex ions with ten isomeric disaccharides through electrospray ionization. The complex ions were further isolated and irradiated by IR and UV lasers separately or continuously in the FTICR cell. Results By combining the two complementary fragment spectra generated from the IR and UV lasers, a clear identification of all the ten isomers was achieved using their binary codes based on their fragmentation patterns. The double-beam method simplifies the experiment by introducing the two lasers sequentially in one experiment, providing richer fragmentation patterns and making the full discrimination easier. Conclusions This study demonstrates the capabilities of the combination of IR and UV photodissociation MS in the identification of diverse glycan isomers. The double-beam photodissociation method described here distinguished compositional, configurational and connectivity disaccharide isomers successfully. Compared with the data accumulation method based on separate IR and UV experiments, this method is simpler, faster, more flexible and also characterized by richer fragmentation patterns.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 5
·056523
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IF 4.386
Chuanhui Zhu,Guo-Hong Cai,Chongyang Yuan,Bin Huang,Guangqin Li,Mark Croft,Martha Greenblatt,Man-Rong Li
Exploring a simple model system to realize the intrinsic guidelines of activity for oxide electrocatalysts is urgent and important. Here, we introduce delafossite oxides A2IrO3 (A = Li, Na, Cu) as a family of oxygen evolution reaction electrocatalysts in alkaline media. We show that, in Cu2IrO3, the intrinsic intersite charge transfer between Cu and Ir improves the electrocatalytic activity by simultaneously increasing the conductivity and reducing the Tafel slope down to 51 mV dec−1 with an overpotential η10 = 361 mV. Through a comparative study, the improved activity of Cu2IrO3 is attributed to the increase of Ir 5d projected electronic density of states with extended Ir–O bond length. This study provides insights into advanced catalyst design through tailoring the active site of oxides by the modulation of electronic states in a given structural motif.
研究领域:
材料科学
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电化学
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催化科学
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Asia-Pacific Journal of Chemical Engineering
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2024
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IF 1.4
Chaoran Zhou,Zhixian Liang,Hao Qiu,Shanshan Jiang,Wei Wang,Chao Su
Solid oxide fuel cells (SOFCs) as highly effective energy conversation devices have gained substantial recognition and research interest. The electrochemical properties of the traditional SOFCs are restricted by the sluggish reaction kinetics for the cathode material when lowering the operation temperature to below 600°C. In addition, the stability of the cathode at reduced temperatures is also a big challenge for the widely popularization of SOFC technology. Achieving high activities and stable ORR in the cathode is crucial for the development of SOFCs. The doping active metal method has been demonstrated as an effective approach to optimize the phase structure and improve the ORR activity of the cathode. Herein, we successfully develop an Ir-doped SrCoO 3 − δ (SrCo 0.98 Ir 0.02 O 3 − δ , SCI) cathode for SOFCs. SCI exhibits a low area-specific resistance (ASR) of 0.057 Ω cm 2 at 650°C, ~ 44% lower than 0.102 Ω cm 2 of Ir-free SrCoO 3 − δ . The Ni–Sm 0.2 Ce 0.8 O 1.90 (SDC) anode-supported fuel cell with SDC electrolyte and SCI cathode obtains an excellent output performance (e.g., 1,128 mW cm −2 at 650°C). The desired results underscore the feasibility of the Ir-doping strategy as an optimized method for the exploitation of advancing cathode in SOFCs.
研究领域:
材料科学
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能源技术
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Meihong Fan,Lijia Liu,Yue Li,Fengyun Gu,Xingquan He,Hui Chen
The industrialization of hydrogen production technology through polymer electrolyte membrane water splitting faces challenges due to high iridium (Ir) loading on the anode catalyst layer. While rational design of oxygen evolution reaction (OER) electrocatalysts aimed at effective iridium utilization is promising, it remains a challenging task. Herein, we present exfoliated Ti 3 C 2 T x MXene as a highly conductive and corrosion-resistant support for acidic OER. We develop an alcohol reduction method to achieve uniform and dense loading of ultrafine Ir nanoparticles on the MXene surface. The IrO 2 /TiO x heterointerface is formed in situ on the Ir@Ti 3 C 2 T x MXene surface, acting as a catalytically active phase for OER during electrocatalysis. The electron interactions at the IrO 2 /TiO x heterointerface create electron-rich Ir sites, which reduce the adsorption properties of oxygen intermediates and enhance intrinsic OER activity. Consequently, the prepared Ir@Ti 3 C 2 T x exhibits a mass activity that is 7 times greater than that of the benchmark IrO 2 catalyst for OER in acidic media. In addition, the /Ti 3 C 2 T x MXene support can stabilize the Ir nanoparticles, so that the stability number of Ir@Ti 3 C 2 T x MXene is about 2.4 times higher than that of the IrO 2 catalyst.
研究领域:
材料科学
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电化学
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催化科学
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Journal of Physical Chemistry C
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2024
·
IF 3.3
Da Shu,Ruipeng Fan,Songyou Yao,He Jiang,Xiaoyue Zhang,Yue Zheng
Understanding the rotor dynamics within metal–organic frameworks (MOFs) is fundamental to the desired amphidynamic application. However, in-depth investigation has been hindered due to the inadequacy of current characterization tools. In this paper, a technique based on infrared-combined atomic force microscopy (AFM-IR) was developed, in which the infrared spectrum can be obtained under tip bias and tip force with nanometer resolution. The tip bias induced variation in infrared spectra of the Cu2(fbdc)2(dabco) film demonstrates that full width at half-maximum of the vibration–rotation coupling mode is competent for rotor speed characterization. Stalling of dipolar rotor speed in the Cu2(fbdc)2(dabco) film is observed under both tip bias and tip force, which indicates the electrical and mechanical controllability of MOF rotor dynamics. On this basis, the rotor behavior of few-layer MOF films is investigated to reveal the influence of self-assembled molecule stress on rotor dynamics. It is found that the rotor rotation is activated progressively as the film grows and self-assembled molecule stress releases. Our results pave the avenue for direct study of rotor dynamics within MOF films at the nanoscale.
研究领域:
材料科学
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化学
·
物理学
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Inorganic Chemistry Frontiers
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2025
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IF 6.4
Yijun Xiang,Hui Wang,Shaoxiong Li,Linlin Li,Jianwei Ren,Gengyu Xing,Liming Deng,Shengjie Peng
Developing stable and efficient single-atom electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for advancing proton exchange membrane water electrolysis (PEMWE). However, the lack of precisely tailored coordination environments capable of preventing Ir single-atom dissolution remains a critical barrier. Herein, we construct Ir single-atom catalysts supported on Co3O4 (IrSA-Co3O4) via the synchronized formation of Co defects and the immobilization of Ir single atoms during precursor pyrolysis. Atomically dispersed Ir atoms are anchored at octahedral Co defect sites, forming a configuration of single atoms confined within the spinel lattice. Benefiting from the oxygen-bridged electronic coupling within the Ir–O–Co configuration, the electronic structure of Ir sites is optimized to enable moderate intermediate adsorption while mitigating dissolution. As a result, IrSA-Co3O4 achieves a low overpotential of 199 mV at 10 mA cm−2 in 0.5 M H2SO4 and operates stably for 150 h at 200 mA cm−2 during PEMWE. This work provides new insights into the rational design of stable single-atom catalysts for acidic OER by effectively suppressing active-site dissolution.
研究领域:
电催化
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材料科学
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能源化学
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纳米材料
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电化学水裂解
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Nature Communications
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2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Wang Dawei,Lin Fangxu,Luo Heng,Zhou Jinhui,Zhang Wenshu,Li Lu,Wei Yi,Zhang Qinghua,Gu Lin,Wang Yanfei,Luo Mingchuan,Lv Fan,Guo Shaojun
Using metal oxides to disperse iridium (Ir) in the anode layer proves effective for lowering Ir loading in proton exchange membrane water electrolyzers (PEMWE). However, the reported low-Ir-based catalysts still suffer from unsatisfying electrolytic efficiency and durability under practical industrial working conditions, mainly due to insufficient catalytic activity and mass transport in the catalyst layer. Herein we report a class of porous heterogeneous nanosheet catalyst with abundant Ir-O-Mn bonds, achieving a notable mass activity of 4 A mg Ir −1 for oxygen evolution reaction at an overpotential of 300 mV, which is 150.6 times higher than that of commercial IrO 2 . Ir-O-Mn bonds are unraveled to serve as efficient charge-transfer channels between in-situ electrochemically-formed IrO x clusters and MnO x matrix, fostering the generation and stabilization of highly active Ir 3+ species. Notably, Ir/MnO x -based PEMWE demonstrates comparable performance under 10-fold lower Ir loading (0.2 mg Ir cm −2 ), taking a low cell voltage of 1.63 V to deliver 1 A cm −2 for over 300 h, which positions it among the elite of low Ir-based PEMWEs.
研究领域:
材料科学
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能源技术
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APPLIED SURFACE SCIENCE
·
2018
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IF 4.439
Zengbo Ke,Lejing Li,Qiurong Jia,Yangong Yang,Hongwei Cui
Au/Ir bimetals are not easy to obtain because alloy phase diagrams are not available for these material combinations (Ronald et al., 2004). Herein, the Au/Ir nanochains (Au/Ir NCs) are synthesized via one-pot, hydrothermal method . By virtue of jagged surface with abundant atomic defects, the Au/Ir NCs are demonstrated much more active than commercial IrO 2 electrocatalysts for oxygen evolution reaction under alkaline media. The potential of the Au/Ir NCs sustains 1.53 V vs reversible hydrogen electrode (RHE) with no obvious decease under current density at 10 milliamps per square centimeter, while that of IrO 2 increase to 1.65 V vs RHE after stability tests for ca. 32 h. The durability as well as the activity of Au/Ir NCs is attributed to the electronic interaction between Au and Ir, which is confirmed by X-ray photoelectron spectroscopy (XPS).
研究领域:
材料科学
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电化学
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QUIMICA NOVA
·
2021
·Vol. 44
·期 1
·58-63
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IF 0.961
Tang Shiyun,Yang Song,Tan Sheng,Guo Junjiang,Tang Anjiang
Qualitative and quantitative assessment of total sulfur and sulfur species in solid phase is necessarily important for development of effective desulfurization methods, reduction of environmental pollution, and prevention of catalyst poisoned. In this work, TPO-IR (Temperature Programmed Oxidation- Infrared) method was used for rapid determination of sulfur species in solid minerals. The high purity of Ag2S was used as the calibration materials at the fixed temperature of 1100 °C, and the TPO experimental runs were performed on the solid minerals of phosphorite and coal. The results show that pyrite sulfur with Tmax of 426 °C, and two thiophene sulfurs with Tmax of 450 °C and 481 °C were found in Kaiyang phosphorite by fitting the TPO-IR curves; while pyrite sulfur with Tmax of 432 °C, complex sulfide with Tmax of 679 °C and sulfate sulfur with Tmax of 939 °C were found in Weng’an phosphorite. For Gas coal, the TPO-IR curves of sulfur release can be deconvoluted into seven individual curves, while that of Anthracite deconvoluted into four individual curves. In conclusion, the TPO-IR method has many advantages for determination of sulfur species in solid phase systems, such as less sample consumption, simple pretreatment, convenient operation and low cost, etc.
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Nature Communications
·
2026
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IF 15.7
Zhou Fengxian,Yang Yingguo,Feng Kai,Hu Zhiping,Wang Pengwei,Luo Ran,Wu Daofu,Zhang Zeyu,Liu Zhengzheng,Xue Zixiao,Ou Zeping,Sun Kuan,He Jin,Du Juan
Recent breakthroughs in three-dimensional (3D) printing of glass have enabled precise shaping of glass structures from macro to microscale while retaining their excellent physical and chemical properties. However, current functional developments in 3D printed glass primarily focus on leveraging its intrinsic optical transparency, with limited exploration of photonics application. 3D-printed glass functionalized by quantum dots (QDs) will hold great promise for creating desired photonic functional macro- and microstructures. However, voxel-precision customization of photonic functions in 3D printed glass by the monodispersed and size-controlled QDs is fundamentally conflict with the high-temperature sintering process required in 3D printed glass. Here, we present a simple, cost-effective method for creating a library of QDs functionalized 3D-printed glasses with tunable UV-VIS-IR photoluminescence (PL) by printing nanoporous glass (NG) followed by low-temperature nanoscale engineering of QDs growth. The integration of uniform and size-controlled QDs imparts 3D printed glass with fine tuning in composition, architecture, and photonic functionalities, while nanoscale engineering of the micro-environment enables precise tailoring of various QDs with enhanced optical performance and stability. This universal approach establishes a benchmark for 3D-printed functional glasses with advanced photonic capabilities.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
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IF 9.6
Shengqin Guan,Baoen Xu,Xingbo Yu,Baixin Han,Binbin Zhang,Taotao Guan,Yu Yang,Kaixi Li,Jianlong Wang
The sluggish kinetics of oxygen evolution reaction (OER) is one of the critical challenges for electrochemical water splitting. Rational design of single atom on metal-support interactions (MSI) using deposition method is essential for electrocatalytic materials. Herein, we report the single-atomic-site and cluster-site iridium stabilized on high-entropy oxides (FeCoNiCrMoO x ) with deposition method using choline chloride/urea deep eutectic solvent (ChCl/U). The resulting Ir single atoms and clusters exhibit an average interatomic distance of approximately 0.77 nm. Ir 1&n -FeCoNiCrMoO x delivers an ultralow overpotential of 193 mV at a current density of 100 mA·cm −2 , and a long-term stability over 240 h for OER by precisely regulating the local coordination environments of the active sites in catalyst. DFT calculations reveal that closely distance single atoms and clusters exhibit stronger interactions with the high-entropy substrate. These strong interactions lead to a shift in the rate-determining step, and Ir 1&n -FeCoNiCrMoO x demonstrates the lowest theoretical OER overpotential. This work introduces DES as an effective electrochemical deposition method with synthesizing closely spaced single atoms and clusters for superior OER activity.
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AICHE JOURNAL
·
2026
·
IF 4.4
Shenhui Yu,Xingfen Huang,Xingyue Shi,Nemin Yang,Bangban Zhu,Haitao Wang,Jieyuan Zheng,Shengbin Shi,Deliang Wang,Qingyue Wang,Khak Ho Lim,Xuan Yang,Pingwei Liu,Wen-Jun Wang
Mechanistic understanding of polymerization kinetics at elevated pressure requires quantitative, time-resolved access to reaction dynamics. Herein, we developed an integrated framework coupling in situ high-pressure ATR-IR spectroscopy with a kinetic model based on the method of moments. Using ethylene/maleic anhydride (E (1)/MAH (2)) copolymerization as a benchmark, this platform enabled real-time quantification of monomer consumption and in situ determination of copolymer composition, directly confirming strict alternating incorporation. The kinetic model showed excellent agreement with experiments, with deviations below 10%. Analysis revealed the cross-propagation of MAH to ethylene-terminated radicals ( k 12 ≈ 5.62 × 10 3 L mol −1 s −1 ) is over an order of magnitude faster than the reciprocal step ( k 21 ≈ 3.92 × 10 2 L mol −1 s −1 ), identifying the latter as rate-determining. Extrapolation of the model guided the precise synthesis of a high-molecular-weight copolymer ( M w = 107 kDa). This work establishes a generalizable in situ platform for elucidating kinetics in complex polymerization systems at elevated pressure.
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