Journal of Materials Chemistry A
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2024
·
IF 10.7
Xu Yu,Han Tian,Ziyi Yu,Fantao Kong,Chang Chen,Ziwei Chang,Jian Huang,Xiangzhi Cui,Jianlin Shi
Hydrogen spillover effect-based active catalyst design is an effective strategy to enhance the hydrogen oxidation reaction (HOR) performance, which, unfortunately, still suffers from the high hydrogen spillover energy barrier. Here, a strategy alloying Ir with Ru is proposed to modulate the electronic structure of Ir to accelerate the H* transfer by a novel Ir–Ru–WO2.72 bridge, thus significantly reducing the hydrogen spillover energy barrier from Ir to WO2.72. The IrRu nanoclusters were deposited on a three-dimensional ordered macroporous WO2.72–C framework, and thus the constructed IrRu–WO2.72–C (1.16 wt% Ir and 1.09 wt% Ru) catalyst exhibits excellent HOR and CO-tolerance performance, rather high cell power density, and especially, 4 times higher mass activity than that of Pt/C. The modulation of Ru largely decreases the work function difference between the IrRu clusters and substrate, resulting in a reduced hydrogen spillover barrier via the Ir–Ru–WO2.72 bridge, weakened CO adsorption and fast removal of the adsorbed CO.
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高影响因子
FUEL
·
2022
·
IF 8.035
Xiaojun Dai,Yan Cheng,Meng Si,Qiang Wei,Dongdong Chen,Wenbin Huang,Yasong Zhou
A series of SAPO-11 molecular sieves were synthesized in the concentrated gel system by reducing the water content in the synthesis system. With SAPO-11 molecular sieves as supports, NiW-supported catalysts were prepared for the hydroisomerization of n-hexadecane. SAPO-11 molecular sieves and catalysts were characterized by XRD, SEM, N 2 adsorption–desorption, NH 3 -TPD, Py-IR, HRTEM and XPS. The results showed that reducing the water content in the synthesis system could increase the mesoporous volume of SAPO-11 molecular sieve and improve the acidity of SAPO-11. For the corresponding catalysts, using SAPO-11 synthesized in concentrated gel system as the support weakened the interaction between the active phase and the support, and increased the dispersion and stacking number of the active phase, which effectively improved the catalytic performance of the catalyst. The yield of i-hexadecane of the catalyst NiW/45W-SA corresponding to SAPO-11 synthesized in conventional water content system was 28.14%, while that of the catalyst NiW/5W-SA corresponding to SAPO-11 synthesized in concentrated gel system was 52.24%. According to the distribution of isomers, it is inferred that hydroisomerization of n-hexadecane over NiW/SAPO-11 follows the pore-mouth mechanism.
研究领域:
催化
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材料科学
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化学工程
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Nanoscale
·
2019
·Vol. 11
·期 48
·23206-23216
·
IF 6.97
Tao Yang,Yihui Wang,Wenxian Wei,Xinran Ding,Maoshuai He,Tingting Yu,Hong Zhao,Dongen Zhang
Fuel cells are expected to be one of the most promising alternatives to the increasingly scarce fossil fuels, and Pt is the most commonly used catalyst for anodic and cathodic electrochemical reactions. To realize large-scale commercialization, it is most urgent to improve the efficiency of Pt and reduce the cost. Here, we synthesized an octahedral Pt–Ni–Ir yolk–shell catalyst through stepwise co-deposition (SCD), surface-limited Pt deposition (SLPD) and Ni-coordinating etching (NCE) processes. Experimental studies showed that the catalytic activities of the as-prepared trimetal yolk–shell catalyst were several times higher than that of the commercial Pt/C towards oxygen reduction and methanol oxidization under both acidic and alkaline conditions. This work may be extended to designing other multimetallic functional materials with complex hierarchical nanostructures, which is conducive to greatly enhancing the performance.
研究领域:
材料科学
·
电化学
·
催化作用
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高影响因子
Journal of Advanced Research
·
2026
·
IF 17.1
Sumei Ling,Yang Xu,ZhouJie Xu,Xiaoli Li,Linfang Lu,Menghan Sun,Wenjun Yang,Yuxuan Liu,Jun Yuan,Shihua Wang
Introduction Sulfamethazine (SM2) antibiotic residues in food pose a significant risk to human health, including pathogenic bacterial resistance, allergic reactions, and carcinogenicity. Current lateral flow immunoassay (LFIA) typically employing colloidal gold (AuNP) as a signal reporter exhibits unsatisfactory sensitivity. Recently, metal–organic frameworks (MOFs) nanomaterial as a supporting matrix for loading nanoparticles provides a powerful tool to improve the performance of LFIA. Objectives This study aims to develop an enhanced immunosensor based on antibody labeled Au/Ir@Cu/Zn-MOF signal amplification nano-composite for sensitive and point-of-care monitoring of SM2 antibiotic residues. Methods Firstly, the highly specific monoclonal antibody (mAb) against SM2 belonging to the IgG1 subclass was screened. Subsequently, the Au/Ir@Cu/Zn-MOF nanocomposite was synthesized by incorporating Au/Ir bimetallic nanoparticles into the previously prepared Cu/Zn-MOF composite. The anti-SM2 mAb was then conjugated to Au/Ir@Cu/Zn-MOF nanocomposite via a co-precipitation method to fabricate the mAb-Au/Ir@Cu/Zn-MOF probe. Finally, a lateral flow immunoassay was constructed for the detection of SM2 residues. Results The vLOD the Au/Ir@Cu/Zn-MOF-based LFIA for SM2 detection was approximately 2.5 ng/mL, which was at least 600 times greater than that of the AuNP-based LFIA (with the vLOD of 1563 ng/mL). Average recovery rates were 80.08–90.8% in milk sample, 88–89.3% in eel sample and 85.3–95.2% in pork sample, respectively. Conclusion The Au/Ir@Cu/Zn-MOF nanocomposite utilized as signal amplification probe demonstrated remarkable sensitivity for the detection of SM2. The developed Au/Ir@Cu/Zn-MOF-based LFIA exhibits significant potential for the rapid and sensitive detection of contaminants in environmental monitoring and food safety.
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ACS Catalysis
·
2026
·
IF 13.6
Peiyun Zhou,Shihao Feng,Xi Wang,Xiang Liu,Xingjian Xu,Xiubing Huang,Haohong Duan
Despite the practical advantages of conducting 5-hydroxymethylfurfural (HMF) electrooxidation to 2,5-furandicarboxylic acid (FDCA) in acidic media, such as facilitated product separation and improved reactant stability over alkaline environments, the lack of efficient electrocatalysts has hindered the development of efficient acidic processes. Herein, we reveal that HMF oxidation reaction (HMFOR) shares key oxygen-containing intermediates ([O], e.g., *OH and *OOH) with oxygen evolution reaction. By incorporating Ir into manganese oxide (MnOx), the kinetic constraints of acidic HMFOR were successfully broken. Specifically, in the designed Ir-MnOx, the presence of Ir sites not only accelerates the generation of [O] species to provide abundant oxidative active species but also modulates the electronic structure of Mn sites to activate their reactivity and enhance HMF adsorption. Synergistic cooperation between Ir and Mn sites endows Ir-MnOx with a record-high HMFOR current density (56.2 mA cm−2@1.40 VRHE), along with high FDCA selectivity (94%) and yield (92%) in an acidic electrolyte (pH 1.89). This work provides mechanistic insights and a design strategy for efficient HMFOR electrocatalysts in acidic environments.
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JOURNAL OF MOLECULAR STRUCTURE
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2012
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IF 1.634
Fu Liu,Zhongbo Wei,Liansheng Wang,Zunyao Wang
4,4′-Dihydroxydiphenyl ether and 4,4′-oxybis(1-methoxybenzene) are synthesized. Experimental and theoretical studies on molecular structure, infrared spectra (IR), Raman spectra and nuclear magnetic resonance ( 1 H NMR) chemical shifts of the two synthesized compounds have been worked out. All the theoretical results, which are obtained with B3LYP/6-311G(d,p) method by using the Gaussian 09 program, have been applied to simulate molecular structure, infrared, Raman and NMR spectra of the compounds. The compared results reveal that the calculated geometric parameters match well with experimental values; the scaled theoretical vibrational frequencies are in good accordance with observed spectra; and computational chemical shifts are consistent with the experimental values in most part, except for some minor deviations. These great coincidences prove that the computational method B3LYP/6-311G(d,p) can be used to predict the properties of other similar materials where it is difficult to arrive at experimental results.
研究领域:
化学
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理论计算化学
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光谱学
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Yi-Heng Wang,Yang Liu,Jin Tong,Shu-Yan Yu
The cyclometalated Ir(III) complex, Ir(ppy) 2 (phen-dipzH 2 ) ( Ir-1 ), was synthesized using the ligand 3,8-di(1H-pyrazol-4-yl)-1,10-phenanthroline (phen-dipzH 2 ) and the auxiliary ligand 2-phenylpyridine (ppy). Crystal structure analysis reveals that each {Ir(ppy) 2 } + unit is coordinated by a neutral phen-dipzH 2 ligand in Ir-1 . The packing arrangement of Ir-1 displays aromatic stacking interactions and [C–H…N] hydrogen bonding interactions between the [Ir(ppy) 2 (phen-dipzH 2 )] + cations. In solution, Ir-1 exhibits emission switching induced by acid/base changes, with the emission wavelength shifting from 562 nm (yellow color) in the neutral state to 618 nm (pink color) under acidic conditions and to 528 nm (gray color) under basic conditions. These shifts are attributed to the protonation and deprotonation of the pyrazole units, which is confirmed by 1 H NMR spectra. Additionally, Ir-1 demonstrates high selectivity and sensitivity toward Cu 2+ ions, with a detection limit as low as 9.47 μM compared to other metal ions. The acid/base-responsive phosphorescence of Ir-1 has also been successfully utilized in the development of paper strip-based devices for urea detection.
研究领域:
化学
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材料科学
·
分析化学
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高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 7
·1834-1846
·
IF 5.686
Ruihuan Jiang,Shaomian Liu,Liang Li,Yongjun Ji,Huifang Li,Xiangfeng Guo,Lihua Jia,Ziyi Zhong,Fabing Su
Graphical Single Ir atoms : In the CO+NO reaction, the catalyst with single-sited Ir atoms (0.28 wt %) anchored on a mesoporous WO 3 (Ir 1 /mesoporous-WO 3 ) showed much higher NO conversion and N 2 selectivity under oxygen-rich conditions than the catalysts supported with Ir nanoparticles on the same catalyst support (Ir NPs/mesoporous-WO 3 ) and on a non-mesoporous WO 3 (Ir/non-mesoporous-WO 3 ). Under oxygen-rich conditions, achieving a selective and efficient reduction of NO by CO is always challenging. Here, we report the synthesis of the catalyst consisting of single Ir atoms anchored on mesoporous WO 3 (denoted as Ir 1 /m-WO 3 ) using a facile template method followed by wet impregnation. X-ray diffraction and transmission electron microscope studies indicated that the Ir atoms were distributed uniformly on the internal surface of m-WO 3 . When tested for the reduction of NO by CO, the Ir 1 /m-WO 3 catalyst with a low Ir loading of 0.28 wt % exhibited excellent catalytic performance in the presence of 2 vol % O 2 (volume ratio of CO to O 2 being 1 : 10), achieving a NO conversion of 73 % and N 2 selectivity of 100 % at 350 °C. In particular, its turnover frequency (TOF) value reached 0.30 s −1 at 200 °C, which is six times higher than that of the catalyst with Ir nanoparticles supported on mesoporous WO 3 (0.05 s −1 ). The superior catalytic performance of Ir 1 /m-WO 3 is attributed to the formation of the isolated Ir atoms and the more newly generated Ir-WO 3 interfaces that can promote the adsorption and activation of NO, and the presence of accessible mesopores in m-WO 3 that facilitates the mass transfer of NO and CO. This study brings a new fundamental understanding of active sites in Ir-based catalysts for the CO+NO reaction and provides a new way to the design and synthesis of single-atom catalysts, especially precious metal catalysts for emissions control.
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JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Wenxiu Cao,Lu Lin,Haifeng Qi,Qian He,Zhijie Wu,Aiqin Wang,Wenhao Luo,Tao Zhang
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction for the production of renewable chemicals and fuels, wherein acid-resistant and robust catalysts are highly desired for practical usage. Herein, an ultra-stable 0.6 wt% Ir@ZrO 2 @C single-atom catalyst was prepared via an in-situ synthesis approach during the assembly of UiO-66, followed by confined pyrolysis . The Ir@ZrO 2 @C offered not only a quantitative LA conversion and an excellent GVL selectivity (>99%), but also an unprecedented stability during recycling runs under harsh conditions (at T = 453 K, P H2 = 40 bar in pH = 3 or pH = 1 aqueous solution). By thorough spectroscopy characterizations, a well-defined structure of atomically dispersed Ir δ+ atoms onto nano-tetragonal ZrO 2 confined in the amorphous carbon was identified for the Ir@ZrO 2 @C. The strong metal-support interaction and the confinement of the amorphous carbon account for the ultra-stability of the Ir@ZrO 2 @C.
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DALTON TRANSACTIONS
·
2013
·Vol. 42
·期 18
·6478-6488
·
IF 3.806
Lihua Ma,Song Guo,Jifu Sun,Caishun Zhang,Jianzhang Zhao,Huimin Guo
Naphthalenediimide (NDI) was connected to the ligand of a cyclometalated Ir(III) complex (Ir-1) via a CC triple bond to enhance the absorption in the visible region and to access long-lived triplet excited states. Ir(ppy)2(bpy)[PF6] (Ir-2, ppy = 2-phenylpyridine and bpy = 2,2′-bipyridine) was used as a model complex. The photophysical properties of the complexes were studied with steady state and time-resolved spectroscopy. Ir-1 shows strong absorption in the visible region (ε = 11 000 M−1 cm−1 at 542 nm) and in comparison Ir-2 shows typically weak absorption in the visible region (ε < 3000 M−1 cm−1 above 400 nm). Room temperature near IR emission at 732 nm (ΦP = 0.1%) was observed for Ir-1, which is attributed to the NDI localized emissive triplet excited state, by transient absorption spectra and DFT calculations on the spin density surface. The lifetime of the NDI-localized triplet excited state is up to 130.0 μs, which is rarely reported for Ir(III) complexes. In comparison, Ir-2 shows phosphorescence at 578 nm and the triplet state lifetime is a typical value of 0.3 μs. The complexes were used as triplet photosensitizers for triplet–triplet annihilation (TTA) upconversion and an upconversion quantum yield of 6.7% was observed with Ir-1. No upconversion was observed with Ir-2 as the triplet photosensitizer at the same experimental conditions.
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Journal of Materials Chemistry A
·
2016
·Vol. 4
·期 47
·18354-18365
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IF 8.262
Lin Han,Pengfei Wang,Hui Liu,Qiangqiang Tan,Jun Yang
Tailoring the internal structure and chemical composition of nanomaterials is an effective way to enhance their performance for a given application. Herein, we report a general wet-chemistry approach to produce copper (Cu)-based binary hollow nanostructures with well defined architectures and investigate their catalytic properties in electrochemical reactions. This strategy relies on the galvanic replacement between Cu seeds and noble metal precursors including ruthenium (Ru), rhodium (Rh), palladium (Pd), osmium (Os), iridium (Ir), and platinum (Pt) in oleylamine at an appropriate temperature, which is essential to balance the reduction kinetics of the noble metal precursors by oleylamine during their galvanic replacement with Cu seed particles. Typically, the bimetallic CuPt hollow nanostructures with polyhedral morphologies exhibit enhanced catalytic properties for the oxygen reduction reaction (ORR), while their spherical counterparts obtained at a relatively low temperature show high activity for the methanol oxidation reaction (MOR). In particular, we will also demonstrate a unique application of the CuRu hollow nanostructures in supercapacitors after converting them into binary metal oxides at elevated temperatures in air.
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American Journal of Translational Research
·
2022
·
IF 3.94
Zheng Xu,Luwei Xu,Yuzheng Ge,Hongbin Sun,Jiageng Zhu,Quanliang Dou,Ruipeng Jia
Background: Cabazitaxel has been applied to the treatment of castration-resistant prostate cancer (CRPC), but the molecular mechanism remained to be fully understood. Methods: After treatment with Cabazitaxel alone or in combination with ionizing radiation (IR), CRPC cell viability, proliferation and apoptosis were determined by Cell Counting Kit-8 (CCK-8) assay, colony formation, and flow cytometry, respectively. Tumor volume was measured after the establishment of animal xenograft model. Relative expressions of proteins related to apoptosis (B-cell lymphoma-2 (Bcl-2), Bcl-2-associated X protein (Bax), and cleaved caspase 3) and phosphoinositide 3-kinase (PI3K)/AKT pathway were measured by Western blot, and the phosphorylated-PI3K/PI3K and p-AKT/AKT ratios were determined as well. Results: Cell viability and proliferation were suppressed, and apoptosis was promoted in CRPC cells after Cabazitaxel treatment alone, accompanied with upregulated expressions of Bax and cleaved caspase 3 and downregulated Bcl-2 expression. Also, a single treatment with Cabazitaxel resulted in suppression of PI3K/AKT pathway activation, along with downregulated expressions of p-PI3K and p-AKT and a reduced ratio of p-PI3K/PI3K to p-AKT/AKT. Meanwhile, Cabazitaxel enhanced the effects of IR on suppressing survival and promoting apoptosis in CRPC cells through downregulating Bcl-2 and upregulating Bax and cleaved caspase 3. However, Cabazitaxel suppressed IR-induced PI3K/AKT pathway activation via downregulating p-PI3K and p-AKT, leading to a reduced ratio of p-PI3K/PI3K to p-AKT/AKT. Furthermore, Cabazitaxel further promoted the effects of IR on suppressing tumor growth in vivo . Conclusion: Cabazitaxel inhibited the proliferation and promoted the apoptosis and radiosensitivity of CRPC cells, which is related to the suppression of PI3K/AKT pathway, providing a therapeutic method for CRPC in clinical practice.
研究领域:
肿瘤学
·
分子生物学
·
药理学
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高影响因子
危险品化学品经营许可证（带存储）