CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Yuqing Pan,Zechu Deng,Ning Liu,Chengna Dai,Biaohua Chen
The alkaline hydrogen evolution reaction (HER) suffers from sluggish kinetics, mainly due to the high energy barrier for water dissociation and mismatched adsorption-desorption balance of key intermediates (H* and OH*). To address this challenge, this study employs a dual-functional strategy combining Co doping and in-situ CO regulation to construct a Co-MoS 2 support with abundant sulfur vacancies (Sᵥ). These Sᵥ can efficiently anchor Ru species as highly dispersed, electron-deficient Ru 4+ state, which leads to excellent alkaline HER performance of Ru 8% @Co-MoS 2 -CO by displaying a low overpotential of 46 mV at 10 mA cm −2 and a Tafel slope of 62 mV dec −1 . Combined experimental characterization and DFT (density functional theory) calculations reveals that Co-Sᵥ synergy not only optimizes Ru’s electronic structure with downshift d band center but also finely modulates the electronic properties of adjacent S site, which thereby enables precise tuning of the adsorption/desorption (ADT) behavior of OH* and H*. Meanwhile, the significantly increased electronic density around the Fermi energy (E F ) leads to enhanced efficiently electronic conductivity of Ru 8% @Co-MoS 2 -CO, as also verified by the SECM measurement, which constitutes another key factor leading to its excellent alkaline HER activity. In addition to that, it is also interestingly found that there probably also exists another route for H evolution, wherein the H* can migrate from the S site to the Ru site by crossing a low energy barrier of 0.83 eV and be evolved into H 2 by following Tafel route, jointly boosting reaction efficiency. Generally, present work provides atomic-scale insights and references for designing high-performance electrocatalysts via defect engineering-regulated metal-support interactions, which would favor other highly-efficient alkaline HER catalyst designs.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Qunwei Guo,Xiaokun He,Jiaqi Geng,Jiawen Pan,Yuan Xue,Nan Xu,Bo Chi,Jian Pu
In this work, Ru is incorporated into Ni/Co to synthesize novel Al 2 O 3 -supported Ni-Ru/Co-Ru bimetallic catalysts. Tests verify their enhanced catalytic capability and durability and also reveal how each catalyst is deactivated. SEM and EDS results indicate that nanoparticle agglomeration on Ni-based surface triggers deactivation, and TG and XPS results suggest carbon deposition is fatal to Co-based catalysts. Implementing Ru effectively enhances catalytic activity and durability. To gain insight into the promoting effect of Ru, quantum mechanical methods are utilized to investigate the shifts in activation energies (E a ) in CH x * dehydrogenation processes on (1 1 1) surfaces. For the Ni catalyst, DFT calculations indicate that adding Ru decreases E a yet does not change the determining step. In contrast, adding Ru on the Co surface changes the major intermediates from CH* to CH 2 *, which inhibits further dehydrogenation , and hence mitigates carbon deposition to preserve the catalytic activity of the surface.
研究领域:
催化化学
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材料科学
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化学工程
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量子化学
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能量转换
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Surfaces and Interfaces
·
2022
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IF 6.137
Weiquan Li,Die Hu,Ke Yin,Chenglong Yu,Bichun Huang
A series of hierarchical Ru-Ce/H-ZSM-5 were designed and synthesized using the sol-gel method, and they were applied as catalysts for the catalytic combustion of chlorobenzene. The pore diameter of the catalyst was adjusted using an amount of sodium alginate (SA). Among all of the catalysts synthesized, the 0.8 wt.%Ru-10 wt.%Ce/H-ZSM-5 catalyst with a crystallization recipe of 1SiO 2 : 0.02Al 2 O 3 : 0.15TPAOH: 0.04SA: 40H 2 O (named RCZA-0.04) exhibited the optimal catalytic activity, with the 90% conversion of chlorobenzene at 247 °C. In addition, the RCZA-0.04 catalyst maintained superb stability during a long-term reaction at 325 °C. The results of characterizations demonstrated that RCZA-0.04 possessed the largest mesoporous volume, which reduced the diffusion resistance of chlorobenzene and increased the dispersion of the active components, thereby enhancing the catalytic activities. Moreover, the RCZA-0.04 catalyst possessed a low Brønsted/Lewis ratio, which was conducive to the adsorption of chlorobenzene and the cleavage of the C Cl bond.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhe Li,Jizhao Zou,Tao Liang,Xinrui Song,Zhangjian Li,Jiaming Wen,Minggui Peng,Xierong Zeng,Haitao Huang,Hongliang Wu
Developing heterostructures in nano-electrocatalyst has been demonstrated as a feasible method to enhance electrocatalytic activities for water splitting, since it still remains a grand challenge to develop highly efficient and stable electrocatalysts for both oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) within a wide pH range. Herein, we report a facile pyrolysis strategy of Ru-MOF for rationally constructing ultrasmall Ru@RuO 2 heterostructures, which exhibit extremely remarkable electrocatalytic performance toward both HER and OER in pH-universal electrolytes. Impressively, optimal Ru@RuO 2 -250 achieves ultralow overpotentials for both OER (198 mV, 263 mV and 182 mV @ 10 mA cm −2 in acidic, neutral and alkaline media) and HER (31 mV, 43 mV and 32 mV @ 10 mA cm −2 in acidic, neutral and alkaline media) due to the full exposure of highly active sites, which are derived from the synergism of abundant heterointerfaces, ultrafine heterostructure size and hierarchical porous structure with high surface area. Theoretical calculations reveal the charge rearrangement and electron conduction intensification near Ru-RuO 2 heterointerfaces, the electronic structure changes of the active sites optimize the adsorption behavior toward various reaction intermediates, reducing the activation barriers and speeding up the reaction kinetics. Deservedly, an asymmetric-electrolyte electrolyzer employed with Ru@RuO 2 -250 is assembled to acquire an ultralow applied voltage of 0.79 V at 10 mA cm −2 based on amphoteric water electrolysis (HER in acidic electrolyte while OER in alkaline electrolyte).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhenyu Ding,Zhe Li,Xiaoxue Zhao,Yanrong Miao,Zhenfeng Yuan,Yuanyuan Jiang,Yizhong Lu
Carbon nitride (C 3 N 4 ) nanosheets are known as peroxidase mimics, but the low activity hinders their further application. Embedding active metal nanoparticles onto the C 3 N 4 nanosheets is expected to break this limitation. Herein, highly dispersed ultrasmall Ru nanoparticles are anchored onto the C 3 N 4 through spontaneous redox reaction. The as-obtained Ru-C 3 N 4 exhibits excellent peroxidase-like activity, which can be further regulated by adjusting the loading of Ru nanoparticles on C 3 N 4 . Using Ru-C 3 N 4 as a mimetic peroxidase, a colorimetric sensing method for alkaline phosphatase (ALP) detection is developed based on the inhibitory effect of ascorbic acid produced by hydrolysis of ALP and l -ascorbic acid 2-phosphate (AAP) on the color development reaction of TMB catalyzed by Ru-C 3 N 4 . The sensor exhibits wide linear range and low detection limit for the ALP sensing. Finally, the assay is applied to ALP detection in human serum and satisfactory results are obtained, which provides a promising strategy for colorimetric sensing of ALP.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Qiuhong Wei,Shujun Qiu,Chengwang Yin,Jiaxi Liu,Yongpeng Xia,Xin Wen,Yongjin Zou,Fen Xu,Lixian Sun,Hailiang Chu
Developing high-performance hydrogen generation/storage materials and technologies is an essential step for applying hydrogen-oxygen fuel cells under the background of carbon peak and carbon neutralization strategy. Ammonia borane (NH 3 BH 3 , AB) features a high volumetric and gravimetric density of hydrogen, showing great potential for chemical hydrogen storage. Exploring low-cost and high-efficiency catalysts is an essential prerequisite for hydrogen generation through AB hydrolysis under mild conditions. Herein, with rationally designing Ru/Co metal-organic framework (RuCo-MOF), a series of Co 2 P nanoparticles doping with low-content Ru embedded in nitrogen-doped carbon supported on graphene oxide (Ru-Co 2 P@N-C/GO) were synthesized via a one-pot phosphorization process. Benefiting from the unique structure and the electronic structure regulation of Ru, Ru-Co 2 P@N-C/GO exhibits excellent catalytic performance with an original turnover frequency (TOF) of 347.3 mol H2 mol Ru –1 min –1 and an excellent specific rate ( r B ) of 83,929 mL min –1 g Ru –1 toward AB hydrolysis. This work opens a new avenue toward developing effective and economic catalysts for AB hydrolysis.
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FOOD CHEMISTRY
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2022
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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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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xianda Han,Zhigang Yu,Yangkejia Xiang,Fengqin Li,Xiaoping Tan,Lan Xu,Guiling Zhang
An electrochemical fabrication method of Ru[bpy] 3 2+ @Cu-MOF(-SH)/Au (MOF = metal–organic framework) was developed with a photo/electrochemical information characterization and a DNA-based biosensing validation for the proposed interface. Applying an anodic synthesis method, a modification layer of Ru[bpy] 3 2+ encapsulated with MOF was formed on the Au electrode surface to fabricate an interface with photo/electrochemical dual-signal response. Combining the scanning electrochemical microscopy (SECM) imaging technology with electrochemical and electrochemiluminescence (ECL) detection, the information about the interfacial photo/electrochemical bi-functional properties was explored from three aspects of the parameter variable, intensity variable, and morphology variable. The results show that the effect of parameter variables on the interfacial response follows an “interference effect” mechanism. Under the optimized conditions, the background and the saturation ECL intensities are 610.0 and 24.0 with a quenching efficiency of 96.1% and a detection limit of 30 fM. The saturation current is 48.8 µA with a detection limit of 330.0 nM. Both ECL and electrochemical imaging methods can corroborate each other, validating the logical correlation between the interface fabrication and the response performance in the regional interfacial distribution and laying a methodological foundation for evaluating the interface fabrication quality based on imaging morphology qualitatively. The proposed interface can construct photo/electrochemical dual-signal DNA-based biosensors.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Tixuan Xia,Chunbo Liu,Yang Lu,Wei Jiang,Hongji Li,Yunchao Ma,Yuanyuan Wu,Guangbo Che
Oxygen evolution reaction is one of the core half-reactions in proton-exchange membrane (PEM) water electrolysis, but its slow reaction kinetics has been limiting the overall energy conversion efficiency (e.g., water splitting). It is urgent to develop efficient catalysts for OER in acidic media. At present, Ru-based catalysts have high activity, but their poor stability makes them difficult to be used in acidic oxygen evolution reactions. The involvement of lattice oxygen mechanism (LOM) in the reaction is one of the main causes of instability in Ru-based catalysts. Herein, we synthesized SrRu 0.5 Ir 0.5 O 3 double perovskite by doping Ir into SrRuO 3 . The double perovskite displays an extraordinary OER performance with a low overpotential of 185 mV at 10 mA cm −2 current density and maintains its catalytic stability for over 50 h in 0.5 M H 2 SO 4 . X-ray photoelectron spectroscopy results show that the electronic synergistic effect between Ir and Ru enables the double perovskite materials with high activity. Meanwhile, the double perovskite catalyst inhibits the occurrence of the lattice oxygen mechanism during the OER, which greatly improve the catalytic stability of Ru-based perovskite materials.
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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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Molecular Catalysis
·
2021
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IF 5.062
Wenwei Su,Jingyi Yang,Meng Zhang,Zhipeng Zhao,Jingli Han,Yongpeng Yang,Jing-He Yang,Zhongyi Liu
Liquid organic hydrogen carriers have been recently developed as the promising hydrogen storage materials, which exhibit significant advantages in hydrogen storage and utilization compared with the conventional hydrogen storage systems. Highly active and sable Ru/SiO 2 catalysts for biphenyl hydrogenation to form bicyclohexyl were synthesized through the strong electrostatic adsorption (SEA) method, and the conventional dry impregnation (DI) method was also considered as comparison. X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and H 2 -temperature-programmed reduction characterization techniques were used to investigate the physicochemical properties of the representative catalysts. The results showed that the catalysts synthesized by the SEA method possessed small-sized and well-dispersed Ru nanoparticles (NPs) on the silica support. Especially, 1.5 wt.% Ru/SiO 2 catalyst exhibited excellent catalytic activity, stability and reusability, where the initial turnover frequency (TOF) was 11.9 h −1 , the conversion of biphenyl was up to 99.9%, and the yield of bicyclohexyl reached 99.9% under the mild conditions (90 °C, 1.0 MPa H 2 ). Further density functional theory (DFT) calculations elucidate that the catalyst with small Ru nanoparticle size exhibits higher catalytic activity for biphenyl hydrogenation.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 6
·1-10
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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）