FOOD CHEMISTRY
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2022
·
IF 9.231
Xin Zhang,Li Tian,Zhuo Sun,Qian Wu,Xiangyu Shan,Yingjie Zhao,Ruizhan Chen,Juan Lu
A molecular-imprinted electrochemiluminescence sensor for procymidone (PCM) detection was reported based on Ru(bpy) 3 2+ @ZIF-7. A novel self-accelerated Ru(bpy) 3 2+ @ZIF-7 was prepared by one-step synthesis method, which exhibited high electrochemiluminescence (ECL) emission as a coreactant in the presence of tri- n -propylamine (TPrA). Concretely, ZIF-7 was not only the carrier of Ru(bpy) 3 2+ , but also the co-reaction promoter of Ru(bpy) 3 2+ /TPrA ECL system. The introduction of molecular imprint polymer (MIP) with PCM gave new characteristics of specific recognition of analyte PCM. The change value of ECL intensity (ΔI) was proportional to the logarithm of PCM concentration, with a wide linear range and a low detection limit of 1.0 × 10 −10 to 1.0 × 10 −6 mol L −1 and 2.0 × 10 −11 mol L −1 , respectively. The presented MIP-ECL sensor had high sensitivity, selectivity and stability, and had great potential in the field of food safety detection.
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TALANTA
·
2023
·
IF 6.1
Chen Cui,Xinyao Lin,Jie Lv,Hang Guo,Lu Shen,Guoqiang Xiang,Wenjie Zhao,Dechen Jiang
Designing innovative electrochemiluminescence (ECL) immunosensors is critical for the detection of biomarkers with a low concentration and the precise evaluation of clinical diseases. Herein, a Cu 3 (hexahydroxytriphenylene) 2 (Cu 3 (HHTP) 2 ) nanoflake-based sandwich-type ECL immunosensor was constructed for C-Reactive Protein (CRP) detection. The Cu 3 (HHTP) 2 nanoflake , an electronically conductive metal–organic framework (MOF), has a periodically arranged porous structure with a cavity size of 2 nm, which not only accommodates a large amount of Ru(bpy) 3 2+ but also confines the spatial diffusion of active species. Therefore, the Ru(bpy) 3 2+ -loaded Cu 3 (HHTP) 2 nanocomplex (Ru@CuMOF) as an ECL emitter exhibits an enhanced ECL efficiency. The ECL resonance energy transfer (ECL-RET) was accomplished by combining Ru@CuMOF used as a donor with gold nanoparticles-functionalized graphene oxide nanosheets (GO-Au) utilized as an acceptor. This should be ascribed to the fact that the ECL emission spectrum of Ru@CuMOF shows the strongest signal intensity at 615 nm, overlapping with the absorption spectrum of GO-Au at 580–680 nm. Targeted detection of CRP in human serum samples was achieved by the sandwich-type immunosensor based on the ECL-RET mechanism with a 0.26 pg mL −1 detection limit. The electro-activated hybrids of Cu 3 (HHTP) 2 and ECL emitters provide a new sensing strategy for the high-sensitivity detection of disease markers.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 19
·6336-6346
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IF 6.4
Dong Guo,Chen Chen,Yongqiang Wang,Youke Wang,Conglu Zhang
Two dimensional materials show unique advantages in catalysis. In this work, it was found that melamine could induce the directional growth of cobalt-based catalysts to form an ultra-thin two-dimensional hexagonal nanosheet structure with only 1.5 nm. In addition, these hexagonal nanosheets (HNs) could grow into a microporous structure under high temperature conditions, and the finally formed CoO hexagonal porous nanosheets (HPNs) had a surface area 11.3 times that of the nanoparticles. Embedding 1.25 wt% of monoatomic ruthenium in the CoO HPNs (CoO/Ru1.25% HPNs) allowed the catalyst to have more active charge storage and transfer centers. The results showed that the overpotential of CoO/Ru1.25% HPNs was 64 mV lower than that of CoO nanoparticles at 10 mA cm−2. The Tafel slope of CoO/Ru1.25% HPNs was only half that of CoO nanoparticles, indicating that a small amount of Ru dispersion and the two-dimensional structure control significantly increased the kinetic rate in the oxygen evolution reaction. The DFT results showed that the Ru single atoms in CoO/Ru HPNs (111) possessed the lowest energy barrier (1.19 eV). The Ru single atoms could effectively reconstruct the neighboring localized structure in the formation of ˙OOH, which desirably decreased the free energy of the system.
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ACS Applied Materials & Interfaces
·
2021
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IF 9.229
Yi-Ru Hao,Hui Xue,Jing Sun,Niankun Guo,Tianshan Song,Jiawen Sun,Qin Wang
Designing and synthesizing stable electrocatalysts with outstanding performance for water splitting is an arduous and urgent task. Herein, Ru-anchored CoP embedded in N-doped porous carbon nanocubes (Ru-CoP/NCs) is successfully prepared. The Ru-CoP/NC reveals superior hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) properties and stability under alkaline conditions, and the corresponding overpotentials are 22 and 330 mV at 10 mA·cm–2, respectively. The unique N-doped porous carbon nanocube could boost the conductivity, and the electronic structure of CoP can be adjusted by the anchoring of Ru. Therefore, the strong interaction between Ru atoms and CoP improves the hydrogen adsorption on the catalyst, hence boosting the HER/OER performance of the Ru-CoP/NC catalyst. This work provides a facile method to exploit high-performance catalysts for water splitting.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Xinyu Chen,Chuntao Chen,Majeed Muhammad Amjad,Dongping Sun,Bianjing Sun,Kai Zhang
Ruthenium (Ru)-based electrocatalysts are regarded as promising for applications in hydrogen evolution reactions (HER) due to their suitable metal-hydrogen (M-H) bonding energy. However, the strong affinity for adsorbed hydroxyl groups (OH ad ) leads to the inactivation of Ru active sites, leading to unsatisfactory performance in practical HER applications. Herein, a competitive adsorption strategy for the design of crystalline lattice-confined atomic Ru in Tungsten Carbide Nanoislands is reported. Benefiting from the unique "island–multi-atoms" structural features, Ru/WC x exhibits ultra-high mass activity (6000 mA mg −1 ) and excellent turnover frequency (3.89 H 2 −1 ) at − 100 mV vs. RHE, which is 9.5 and 51.2 times higher than commercial 20% Pt/C, respectively. In-depth mechanistic analysis demonstrates that the strength of Ru-OH ad is regulated by the oxophilicity of W atoms and the stronger W-OH ad bond to alleviate Ru site inactivation, thus enhancing the HER activity. This strategy provides a novel concept for designing advanced catalysts.
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ENERGY CONVERSION AND MANAGEMENT
·
2023
·
IF 10.4
Liangyong Chen,Daocheng Liu,Guoqiang Wei
Integrated Capture and Methanation of CO 2 (ICCM) with H 2 produced from renewable energy is a novel Power-to-Gas technology. The combination of ICCM with CO 2 point source, such as coal-fired power plant, is anticipated, which greatly motivates the investigations into the influences of coal ash on the key performance of dual function material (DFM) used in ICCM process. Via the experimental study on the coal ash impacts, this work explored the adaptability of DFM and ICCM to coal-fired power plant. Na-Ru/Al 2 O 3 DFM and two ashes collected from the electrical precipitators of supercritical coal-fired power plants were used for experiments. It showed that fly ashes contaminated CO 2 adsorbents and active sites of DFMs, and caused successive drops in carbonates conversion and CH 4 selectivity upon cyclic ICCM reactions. The CO 2 -TPD and H 2 -TPSR tests revealed that the declined supply capability of hydrogen atoms by Ru sites, and the increased rate gap between CO formation and the following CO hydrogenation were responsible for the declined methanation ability of ash-contaminated DFMs. The roles of SiO 2 and Fe 2 O 3 phases in ashes were identified, indicating that SiO 2 reacted with adsorbent components and masked Ru sites, and then induced DFM deactivation by affecting the transport processes of key reactants; Fe 2 O 3 successively invaded both Ru sites and Na 2 CO 3 /γ-Al 2 O 3 interface, leading to successive losses in methanation ability and CO 2 desorption capacity with cyclic ICCM reactions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jialin Cai,Wenlei Zhang,Yanyan Liu,Ruofan Shen,Xin Xie,Wanyu Tian,Xingang Zhang,Jie Ding,Yushan Liu,Baojun Li
The development of high-efficiency pH-universal electrocatalyst is of great significance for hydrogen evolution reaction (HER). In this work, a rod-like Ru/WO 3 -V O electrocatalyst was constructed for HER via a solid-phase reaction strategy. Due to the restriction of atomic migration at solid phase interface, plenty of oxygen vacancies (V O ) and structure distortions were generated in amorphous/crystalline WO 3 phase (WO 3 -V O ). The optimized Ru/WO 3 -V O annealed at 450 °C with 2.2 wt % Ru achieves outstanding intrinsic activity with low overpotential and Tafel slope in a 0–14 pH range. A turnover frequency value 7.2 higher than that of commercial Pt/C is abtaind on Ru/WO 3 -V O at overpotential of 100 mV. Density functional theory calculations reveal that H* adsorption and desorption balanced by tuning the interface electronic structure contributes synergistic effect to the pH-universal HER activity of Ru/WO 3 -V O . The crystalline/amorphous semiconductor-metal heterointerface is crucial to designing and synthesizing electrocatalysts for optimal HER activity.
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JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Guangmin Ren,Zehui Zhao,Zizhen Li,Zisheng Zhang,Xiangchao Meng
Herein, we applied a rapid Joule heating method to form oxygen vacancies and further induced the deposition of Ru clusters onto BiVO 4 . The rapid Joule heating method fabricated oxygen vacancy on BiVO 4 , resulting in the formation of electron-rich active Ru sites and unsaturated V sites. The pristine BiVO 4 was almost no activity in photocatalytic ammonia synthesis. The photocatalytic production rate of ammonia was increased to 3.88 μmol g - 1 h -1 after the formation of oxygen vacancies, and further increased to 16.57 μmol g -1 h -1 with Ru clusters loaded on BiVO 4 . It was indicated that unsaturated V sites near the oxygen vacancy and Ru clusters might act as the reactive sites for N 2 adsorption and activation. And the strong metal-support interactions between Ru and BiVO 4 resulted in charge redistribution between Ru clusters and BiVO 4 supports, thus reducing energy barrier of the rate-determining step for the N 2 hydrogenation. Furthermore, DFT confirmed that associative alternating pathway was suitable for this process.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Tiantian Sun,Xinlin Wang,Zhiyao Duan,Qiong Zhang,Yingxiu Zhao,Guang-Rui Xu,Wei Wang,Lei Wang
Efficient and low-cost electrocatalysts for the hydrogen evolution reaction (HER) are required for producing hydrogen energy through water splitting. Carbon materials as HER catalyst supports are explored widely since the strong metal–support interactions are generally believed to be active and stable toward HER. Herein, we report N-doped porous carbon materials as novel substrates to stabilize the cluster metal sites through the Ru(III) polyamine complexes, which play an important role not only in efficient electron transfer but also in the increasing utilization of metallic active sites. Meanwhile, due to the strong metal–support interactions driven by Ru(III) polyamine complexes, the obtained Ru cluster with a mass loading of 3% on N-doped porous carbon nanoplates (Ru cluster@NCs) exhibits robust stability for HER at a constant voltage, proving to be a promising candidate catalyst for HER. Density functional theory calculations further indicate that the Gibbs free energy (ΔG) of adsorbed H* of Ru cluster@NCs is much closer to zero compared to Ru@(10%)NCs and Pt/C(20%), thus Ru cluster@NCs facilitate the HER process.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jinxiu Cai,Lingbo Zong,Kaicai Fan,Fuxiang Song,Jianyang Gao,Zumin Wang,Yanan Chen,Lei Wang
Due to energy crisis and environmental pollution, it is urgent to develop efficient and cheap catalysts for hydrogen production from water electrolysis. As a cheaper platinum group metal , Ru , a cheaper platinum group metal, is a highly competitive candidate to Pt because of the similar bond energy of M-H. Herein, TiO 2 @nitrogen-doped carbon composite supported superfine Ru nanoparticles was synthesized by high temperature shock in a Joule furnace using Ti-MOF support (Ru/TiO 2 @NC-J). In the extremely rapid process, MOF was quickly converted into highly conductive nitrogen-doped carbon with tiny TiO 2 dispersed in it, and superfine Ru nanoparticles were generated simultaneously in less than 0.5 s. The obtained Ru/TiO 2 @NC-J displays wonderful HER performance in the wide pH range. In 1.0 M KOH solution, the overpotential was as low as 11 mV at 10 mA cm −2 and a Tafel slope was 39.2 mV dec −1 , which far exceeded the activity of Pt/C and conventional calcined samples as well as most of the recently reported catalysts. The as-developed electrocatalysts also showed excellent stability to accommodate large working current for long term test without obvious activity loss in universal pH range. Experimental investigations suggest that the strong metal-support interaction dominantly facilitate the activity of electrocatalytic hydrogen evolution reaction (HER), and stability of Ru/TiO 2 @NC-J. This strategy provides a new and super-fast methodology to prepare low-budget and high-performance HER catalysts for practical applications.
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ACS Catalysis
·
2023
·
IF 12.9
Chao Zhang,Yingqiang Li,Yue Xie,Zhanjiang Yu,Xin Wan,Xinzhi Wang,Jiaan He,Junlang Li,Zhenguo Chen,Xiaoyong Li,Xiaohui Yi,Zhaoli Wang,Guang-Guo Ying,Dionysios D. Dionysiou,Mingzhi Huang
Selective hydrodehalogenation and hydrodearomatization of toxic chlorophenols into value-added chemicals represents a grand challenge for their efficient reutilization. For this purpose, single-atom catalysts (SACs) could be a strategy with relatively high catalytic selectivity and atom utilization but suffer from the catalytic limitation caused by low metal loading densities. Graphdiyne and γ-graphyne are considered promising substrates of SACs with excellent catalytic properties. Additionally, their quantum dots with nanometer size are expected to supply numerous surface anchoring sites and large atom spacing to confine metal cations to synthesize high-loading SACs. Here we report a synthesis approach for high-loading Ru SACs anchored on graphdiyne/γ-graphyne quantum dots (GDQD-Ru/GNQD-Ru), which exhibit remarkably higher turnover frequency (TOF) and selectivity (>99%) of hydrodehalogenation and hydrodearomatization of chlorophenols than graphdiyne/γ-graphyne nanosheet-based Ru SACs and nanoparticles. There is no significant selectivity decrease in chlorophenol transformation by GDQD-Ru/GNQD-Ru observed in 5 catalyst reuse cycles. GDQD-Ru/GNQD-Ru contribute to nearly exclusive hydrodehalogenation and hydrodearomatization without altering any other bonds in chlorophenols. Experimental results and theoretical calculations reveal that GDQD-Ru is more prone to lower energies of rate-limiting steps in H2-driven chlorophenol transformation than GNQD-Ru. The results confirm that graphdiyne/γ-graphyne quantum dots play crucial roles in facilitating the metal atom loading of SACs. Ru loadings are 27.6 and 16.0 wt % in GDQD-Ru/GNQD-Ru, approximately 7-fold and 4-fold higher than reported Ru SACs, respectively. This study provides mechanistic insights toward the roles of high-loading Ru SACs on sp- and sp2-hybridized carbonaceous substrates in selective hydrodehalogenation and hydrodearomatization.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 6
·1-10
·
IF 5.833
Zhang Ze,Yu Hongwei,Zhang Yingcong,Wang Zhangmin,Gao Hongmin,Rong Shengzhong,Meng Lingqiang,Dai Jianmin,Pan Hongzhi,Chang Dong
A sandwich-format electrochemiluminescence (ECL) immunosensor has been developed for alpha-fetoprotein (AFP) detection based on the use of ordered mesoporous carbon-molybdenum disulfide (OMC-MoS 2 ) as a sensor platform and cuprous oxide @ ordered mesoporous carbon-Ru(bpy) 3 2+ (Cu 2 O@OMC-Ru) composites as signal tags. OMC alongside MoS 2 plays a synergistic role in improving the electrochemical performance of the electrode in the electron transfer process. The uniform cubic-shaped Cu 2 O@OMC-Ru nanocrystals display excellent luminous efficiency, with a signal amplification strategy of OMC-MoS 2 synergistic enhancement and Cu 2 O@OMC which is capable of immobilizing more Ru(bpy) 3 2+ serving as a tracing tag to label antibodies. A detectable ECL emission at a Cu 2 O@OMC-Ru nanocrystals modified electrode is initiated at an applied voltage of +1.15 V (scanning range: 0–1.2 V), in the presence of the tripropylamine (TPA) as coreactant. With the increase in AFP concentration, the loading of Cu 2 O@OMC-Ru at the electrode increases. Afterward, the ECL detection of AFP shows a wide linear range from 0.1 pg/mL to 10 ng/mL with a correlation coefficient of 0.9964 and a detection limit of 0.011 pg/mL (S/ N = 3) under the optimal experimental conditions. The recoveries were in the range 91.2–97.1% with RSD varying from 4.8 to 8.5%. Overall, the novel immunosensor has been successfully applied to the analysis of human serum samples, indicating a great potential for application in clinical diagnostics. Graphical abstract
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危险品化学品经营许可证（带存储）