INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Gang Huang,Chenggong Wang,Danil Bukhvalov,Yingchun Yang,Jialu Gao,Fengyan Han,Xiaofei Yang,Caiqin Wang
Urea-assisted water electrolysis is a significant and sustainable strategy to optimize electrolyte system to promote the efficiency of hydrogen producing in overall water splitting. Here we construct excellent catalysts (NiCoRu-X) by introducing Ru into reduced dual metal-organic frameworks (MOFs) via a mild chemical reduction method, which preserves multi hetero-interfaces that are spontaneously formed. Interestingly, excellent performances in urea oxidation reaction (UOR) can be observed on all NiCoRu-X samples but without obvious difference in the activity, while the optimal catalyst can be distinguished by testing their catalytic activity in hydrogen evolution reaction (HER). Dependent density functional theory (DFT) calculations are applied to identify the potential activity sites of different heterostructure in NiCoRu-X, and reveal that the hetero-interface promotes the formation of dynamic Ni 3+ actives like NiOOH, which benefit for UOR. In the urea-assisted electrolytes, the reaction potential difference by coupling the LSV curves of HER and UOR is 155 mV lower than that in the electrolyte without urea at 20 mA cm −2 , and 70 mV lower than that in overall water splitting. It reaches a high faraday efficiency (FE) of 98.5 % at 2.0 V in urea-assistant water electrolysers, higher than that without urea assistant (92.9 %). This work highlights the possibility of using urea oxidation to decrease the reaction overpotential and to further improve the efficiency of producing hydrogen in overall water splitting by introducing urea in electrolyte system.
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FOOD CHEMISTRY
·
2026
·
IF 9.8
Ruidan Li,Li Tian,Yujia Song,Yanjia Guo,Guangping Ma,Pengfei Han,Hanyue Jiang,Wenzhuo Wang,Tengying Ma
In this paper, a dual-mode electrochemiluminescence-electrochemical (ECL-EC) sensor was constructed using Ru(bpy) 3 2+ @Ti 3 CN and Zn 4 Sn 3 O 5 via multi-step amplification strategy for the detection of sodium saccharin (SS). The maximum ECL/EC initial signals were obtained by the synergistic action of Ru(bpy) 3 2+ @Ti 3 CN and Zn 4 Sn 3 O 5 in the tri-n-propylamine (TPrA) solution. Given that SS reacted with Ru(bpy) 3 2+ , the ECL/EC signal values both decreased. The relevant mechanism was investigated. Under the best optimization conditions, the ECL detection exhibited a linear range of 5.0 × 10 −15 to 5.0 × 10 −10 mol·L −1 with a limit of detection (LOD) of 1.67 × 10 −15 mol·L −1 (S/N = 3), while EC detection showed a linear range of 5.0 × 10 −9 to 5.0 × 10 −4 mol·L −1 with the LOD of 1.67 × 10 −9 mol·L −1 (S/N = 3). Satisfactory results were obtained in a variety of actual samples.
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CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Yibo Qin,Longfei Chen,Lixia Ge,Yanfeng Zhu,Wanting Li,Xinxin Cao,Tianchang Wang,Jiong Li,Wei Han,Xinqing Chen
Hydrogen spillover plays a crucial role in heterogeneous catalysis, significantly enhancing the activity of catalysts. However, the promotion mechanism of hydrogen spillover on non-reducible oxide supports (such as zeolite) is rarely reported. Herein, we prepared Ru@Beta sample by in-situ approach, effectively encapsulating Ru species into Beta zeolite. Additionally, three samples (Ru/SiO 2 , Ru@Naβ, and Ru@Hβ) with different hydrogen spillover effect were prepared. The optimal concentration of Ru was 0.5 wt%, and the Ru@Hβ sample with the strongest hydrogen spillover has 100 % conversion rate of N-ethylcarbazole (NEC) and 98 % selectivity towards to 12H-NEC. In contrast, the Ru/SiO 2 with weak hydrogen spillover has only 89.5 % conversion rate and 28.9 % selectivity of 12H-NEC. Notably, the Ru@Hβ can still completely convert NEC even after 7 cycles, thereby exhibiting its remarkable activity and stability. Various characterizations (HAADF-STEM, XPS, EXAFS, in-situ DRIFT, and H 2 -TPD) indicate the superior catalytic performance of Ru@Hβ with strong hydrogen spillover effect, originating from the presence of more hydroxyl (–OH) and Brønsted acid on the surface, while Lewis acid act as hydrogen acceptors and NEC hydrogenation sites. This work not only expands our understanding of the hydrogen spillover, but also paves the way onto the potential applications in heterogeneous catalysis for efficient hydrogenation.
研究领域:
催化化学
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材料科学
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能源存储
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Small
·
2025
·
IF 12.1
Hao Wu,Zixin Rao,Yuting Luan,Xiaoyu Jiang,Li Li,Yongfu Lian
Simultaneous control over the size and electronic structure of ruthenium nanoclusters (Ru NCs) is crucial for optimizing their electrocatalytic performance. Herein, this challenge is addressed by systematically screening typical non-metal heteroatoms (e.g., N, P, S, or B) in graphene (G) substrate to mediate the nucleation and growth of Ru NCs. Theoretical analysis identifies S as the optimal candidate mainly by comparing the Gibbs free energy of Ru adsorption. Experimentally, Ru NCs on S-doped G (G-S) exhibit a uniform and dense distribution, with an average diameter of ≈1.1 nm, significantly smaller than those supported on N-, P-, or B-doped G. The resulting Ru/G-S catalyst demonstrates exceptional bifunctional catalytic activity, surpassing commercial Pt/C in both the hydrazine oxidation reaction (HzOR) and hydrogen evolution reaction (HER). Specifically, it requires an ultralow working potential of −46 mV (vs RHE) for HzOR and a minimal HER overpotential of 15 mV at 10 mA cm −2 . In a two-electrode system, it needs only 31 mV to deliver 10 mA cm −2 and maintains stability over 120 h. Mechanistic studies further reveal that S-doping not only dictates Ru nucleation but also induces charge redistribution, lowering kinetic barriers for the formation of key HzOR and HER intermediates.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 25
·2301343
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IF 19
Ping Yan,Tao Yang,Minxi Lin,Yanan Guo,Zipeng Qi,Qiquan Luo,Xin-Yao Yu
Layered metal hydroxides (LMHs) are promising catalysts for oxygen evolution reaction. However, the hydrogen evolution reaction (HER) activity of LMHs is unsatisfactory due to their poor conductivity and limited active sites. Herein, taking Ni(OH) 2 as demonstration, a novel “one stone five birds” plasma activation strategy synergistic with Ru single atoms (Ru SAs) doping is developed to boost the HER activity of Ni(OH) 2 by constructing heterostructured β-Ni(OH) 2 /Ni-Ru SAs nanosheet arrays (NSAs). Benefiting from the structural/compositional features and optimized electronic state, the as-obtained β-Ni(OH) 2 /Ni-Ru SAs NSAs exhibit splendid HER activity with a low overpotential of 16 mV at 10 mA cm −2 and a small Tafel slope of 21 mV dec −1 in alkaline solution. Excellent HER performance in alkaline seawater and neutral solutions are also demonstrated by the β-Ni(OH) 2 /Ni-Ru SAs NSAs. The plasma activation and Ru SAs doping play important roles in enhancing water adsorption and accelerating the kinetics of water dissociation. Density functional theory (DFT) calculations reveal that the introduction of Ru SAs in the system facilitates the generation of surface OH vacancies for providing more active sites as well as decreases the antibonding state density of the generated mid-gap state for enhancing H adsorption strength toward the optimal range.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Zixuan Wang,Yonglong Wang,Juping Wang,Weiping Xiao,Guangrui Xu,Zhenjiang Li,Chunlong Dai,Huadong Zhang,Zexing Wu,Lei Wang
Designing highly efficient catalysts act as a key role for the green and sustainable hydrogen production through water electrolysis. In this work, hollow structured B-doped FeP nanospheres supported Ru (Ru/h-B-Fe-P) is developed by low temperature phosphorization, acid etching and following microwave treatment approach. The hollow structure, abundant defects and electronic interactions between Ru and FeP can favour the mass transport and boosting the reaction kinetics toward all-pH hydrogen evolution reaction (HER). Then, Ru/h-B-Fe-P achieves excellent catalytic activities in acidic, neutral, alkaline, and alkaline seawater electrolytes with only 56 mV, 79 mV, 88 mV and 99 mV to drive 10 mA cm −2 with remarkable stability. This work indicates that decorated noble metals onto specific nanostructured matrix is a promising approach to enhance the catalytic activities.
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Journal of Energy Chemistry
·
2023
·
IF 13.1
Chuan Hu,Fengli Wei,Qinrui Liang,Qiming Peng,Yuting Yang,Tayirjan Taylor Isimjan,Xiulin Yang
The construction of oxide/metal composite catalysts is a competent means of exploiting the electronic interactions between oxide/metal to enhance catalytic activity. In this work, we construct a novel heterogeneous composite (Ru/HfO 2 -NC) with Ru/HfO 2 nanoparticles nested in nitrogen-doped porous carbon via a zeolitic imidazole frameworks-assisted (ZIF) co-precipitation and calcination approach. In particular, ZIF guides an in-situ construction of nested configuration and confines the scattered nanoparticles. Strikingly, Ru/HfO 2 -NC exhibits unusual ORR activity, superb durability, and methanol tolerance in 0.1 M KOH solution with high half-wave potential ( E 1/2 ) of 0.83 V and follows a near-4e − reaction pathway. Additionally, the ZAB assembled with cathodic Ru/HfO 2 -NC outputs a power density of 157.3 mW cm −2 , a specific capacity of 775 mA h g Z n - 1 , and a prolonged lifespan of 258 h at 5 mA cm −2 . Meanwhile, the catalyst has demonstrated potential applicability in flexible ZAB. As suggested by experimental results and density functional theory (DFT) analysis, the remarkable property possibly originated from the optimization of the adsorption and desorption of reactive intermediates caused by the reconfiguration of the electronic structure between Ru and HfO 2 .
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yingqiao Zhou,Yining Liang,Xiaoning Liu,Xinhua Qi
As one of the important value-added chemicals that has wide applications, the catalytic hydrogenation of glucose to sorbitol has been a hot topic in biomass upgrading. In order to support the prosperity of the sorbitol industry, catalysts with superior activity, higher selectivity, longer life, and lower cost are desirable. Herein, tremelliform graphene-like carbon-encapsulated Ru catalysts (Ru/GLC) were synthesized from 4-nitrocatechol by using solvent evaporation-induced self-assembly and KHCO3 chemical activation processes. The Ru/GLC materials were used for the catalytic hydrogenation of glucose to sorbitol, and the best Ru/GLC-600 sample prepared at a 600 °C activation temperature exhibited both high glucose conversion of 100% and sorbitol yield of 96.8% at 140 °C and 3 MPa H2 in 120 min. The Ru/GLC-600 catalyst exhibited excellent stability and durability that sorbitol yield could be remained at 95.4% after recycling five runs. The catalyst was applicable to concentrated glucose solutions (50 wt %) with 95.6% sorbitol yield. Compared with previously reported catalysts, Ru/GLC catalyst had lower apparent activation energy (Ea = 30.66 kJ/mol) and higher turnover frequency (TOF = 1680.6 h–1). This work provides a simple one-pot synthesis strategy for graphene-like carbon materials for metal encapsulating, and the prepared materials exhibited high catalytic activity and stability for glucose hydrogenation to sorbitol.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Luyan Shi,Ke Zhu,Yuting Yang,Yi Liu,Shoulei Xu,Tayirjan Taylor Isimjan,Xiulin Yang
Designing a cost-effective and high-performance catalyst for NaBH 4 hydrolysis is a significant step in developing a sustainable hydrogen source . Herein, we prepared a cost-effective Ru-clusters decorated cobalt-cerium oxides coating ZIF-67 (Ru/Co 6 Ce 1 @ZIF-67) catalyst via a facile reduction method, displaying high performance and exceptional reusability in alkaline NaBH 4 solution. The optimized catalyst exhibits a high hydrogen generation rate (HGR, 5726.1 mL min −1 g −1 ), turnover frequency (TOF, 413.9 mol H2 min −1 mol R u − 1 ), and low activation energy (E a , 53.0 kJ mol −1 ), surpassing most of the recently reported catalysts. Furthermore, the catalytic performance does not change considerably after five cycles, indicating the catalyst's multi-cycle reusability. Studies imply the uniquely synergistic effect of Ru, Co/Ce oxides, abundant oxygen vacancies , as well as the porous nanocube structure, enabling the catalysts to possess high metal dispersion, outstanding catalytic performance and exceptional reusability. This work will open light on using an oxygen vacancies-rich strategy to design a high-activity catalyst for promoting NaBH 4 hydrolysis.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 11
·1-15
·
IF 6.408
Qin Dongmiao,Meng Shuo,Wu Yusheng,Luo Zhi,Deng Biyang
An efficient electrochemiluminescence resonance energy transfer (ECL-RET) method is proposed which combines the luminescent materials of tris(4,4′-dicarboxylicacid-2,2′-bipyridyl) ruthenium(II) (energy donor) and tin dioxide and tin disulfide quantum dots (SnO 2 /SnS 2 QDs) (energy acceptor) into the isoreticular metal − organic framework-3 (IRMOF-3) material to form a composite. In this mode, the distance between the energy donor and the acceptor was greatly shortened, reducing the energy loss, and thereby effectively improving RET efficiency and further significantly improving the ECL signal. The obtained composite (SnO 2 /SnS 2 QDs-Ru@IRMOF-3) was combined with sandwich immunoreaction to construct an ECL immunosensor for the sensitive detection of procalcitonin (PCT). Under the optimized experimental conditions with a working potential of − 1.48 V (vs Ag/AgCl), the proposed PCT biosensor exhibited a linear concentration range of 1 × 10 −4 –200 ng mL −1 , with a detection limit of 0.029 pg mL −1 ( S / N = 3). The biosensor was used to detect PCT in actual samples. The biosensor has broad application prospects in biological analysis and clinical diagnosis due to its high sensitivity, good selectivity, and good stability. Graphical abstract
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Yuting Yang,Yi Huang,Shuqing Zhou,Yi Liu,Luyan Shi,Tayirjan Taylor Isimjan,Xiulin Yang
Surface vacancy defects, as the bridge between theoretical structural study and the design of heterogenous catalysts, have captured much attention. This work develops a metal-organic framework-engaged replacement-pyrolysis approach to obtain highly dispersed Ru nanoparticles immobilized on the vacancy-rich Ni-NiO@C hollow microsphere (Ru/Ni-NiO@C). Fine annealing at 400 °C introduces nickel and oxygen vacancies on Ru/Ni-NiO@C surface, resulting in an improved electrical conductivity and rapid mass-charge transfer efficiency. Ru/Ni-NiO@C with a hollow micro/nanostructure and interconnected meso-porosity favors the maximal exposure of abundant active sites and elevation of hydrogen oxidation reaction (HOR) activity. Experimental results and density functional theory (DFT) calculations reveal that an electronic effect between Ru and Ni-NiO@C, in conjunction with nickel/oxygen vacancies in the NiO species could synergistically optimize hydrogen binding energy (HBE) and hydroxide binding energy (OHBE). The HBE and OHBE optimizations thus created confer Ru/Ni-NiO@C with a mass activity over 7.75 times higher than commercial Pt/C. Our work may provide a constructive route to make a breakthrough in elevating the hydrogen electrocatalytic performance.
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Applied Biological Chemistry
·
2022
·Vol. 65
·期 1
·1-10
·
IF 3.206
Yu Ying,Huan Siqi,Wang Xiaodan,Yang Cong,Liu Dengyong
A sensitive electrochemical sensor for the selective detection of 5ʹ-guanylic acid (5ʹ-GMP) was prepared by combining sulfonated-multiwalled carbon nanotubes (SMWCNTs) and [Ru(bpy)2dpp]Cl2, which were dripped on the surface of a glass carbon electrode (GCE) immobilized with gold nanoparticles. The 5ʹ-GMP electrochemical biosensor was fabricated using [Ru(bpy)2dpp]2+/SMWCNTs/Au/GCE as working, Ag/AgCl as reference and Pt as auxiliary electrode connected by an electrochemical workstation. The modified electrode was characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The results showed the sensor’s response current had the best peak shape and maximum peak when the pH of electrolyte was 3, scan speed of CV was in the range of 100 to 180 mV/s, and the enrichment time was in the range of 200 to 300 s. Under the optimum conditions, a linear analytical curve was obtained for 5ʹ-GMP concentrations in the range of 0.01 to 0.5 mmol L−1, with a detection limit of 0.0014 mmol L−1. The analytical results of the 5ʹ-GMP sensor were exhibited good consistent with the data from liquid chromatography. The sensor has good reproducibility, long-term stability and strong immunity to interference, and may be a powerful device for 5ʹ-GMP detection, with great advantages such as simple preparation and operation, low equipment cost.
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