APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zichen Wang,Suhao Chen,Runzhe Chen,Haoran Jiang,Yinghui Jiang,Qiliang Wei,Wei Wu,Jun Zhong,Niancai Cheng
The sluggish kinetics of the oxygen evolution reaction (OER) caused by the complex process significantly hinder the advancement of electrolytic water to hydrogen technology. Herein, the valence of Ru is modulated and stabilized through inducing the electronic competition between Mo and Ru, and the charge transfer from Fe, Co, and Ni to Ru in 2D porous FeCoNiMoRu high entropy oxides (HEO) nanosheets to achieve efficient and stable OER. The 2D porous structure of FeCoNiMoRu HEO contributes to the high exposure of active sites while promoting rapid mass transfer, which can facilitate oxygen-evolving kinetics of the catalyst. Consequently, the optimized catalyst (FeCoNiMoRu HEO) surpasses RuO 2 (315 mV) in OER catalytic activity, exhibiting an overpotential of 226 mV at 10 mA cm −2 . Notably, the mass activity of FeCoNiMoRu HEO is nearly 18.6-fold that of RuO 2 . Combined experimental and theoretical analysis, a charge competition between Mo and Ru atoms, and the charge transfer from Fe, Co, and Ni elements to Ru in HEO can buffer the change of valence of Ru and modulate its electronic structure, thus enhancing the activity and durability of FeCoNiMoRu HEO during OER.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xiang Xu,Jingxu Tian,Zijie Sun,Kueasook Ratchadaporn,Peng He,Zheng Zeng,Liqing Li
The expensive material costs of precious metals long limit their use as catalysts. The development of High-Entropy Alloy (HEA) materials provides a feasible approach to combine high performance and lower cost. Therefore, Ru-containing HEA nanoparticles are synthesized on carbon nanofibers. Among them, Ru 0.2 @CNFs reveals the best catalytic oxygen evolution reaction (OER) performance and extraordinary stability for the 1000th cycle. Moreover, the Ru-containing multimetallic catalyst models are calculated based on crystal information obtained from X-ray diffraction result. The great electrocatalytic potential of the Ru 0.2 <1 1 1> crystal face is indicated by the density of states and d-band center, which might benefit from the stronger atomic interaction caused by high-entropy mixing. The largest configuration entropy of Ru 0.2 HEA (1.58 R ) gives a reasonable explanation for its remarkable stability in OER electrocatalysis. In addition, the similar adsorption energies of *OH demonstrate the abundant active sites on the surface of RuFeCoNiCu HEA. As a result, the high-entropy material Ru 0.2 @CNFs can provide potential nanocatalysts with reduced noble metal loading for practical applications. Besides, significant insights for performance prediction in other high-entropy materials are given by the modeling and calculations of HEAs.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Yuxin Sun,Yunshuo Wu,Haiqiang Wang,Zhongbiao Wu
Nitrous oxide (N2O) has gained increasing attention as a potent greenhouse gas, and its catalytic decomposition offers a promising mitigation strategy. In this study, single-atom Ru embedded in a rod-shaped CeO2 catalyst was synthesized via a H2O2 chemical etching strategy. The single-atom Ru catalyst demonstrated an exceptional N2O decomposition performance with only 0.48 wt % Ru loading, exhibiting a 34-fold increase in the turnover frequency compared to Ru nanoparticle catalysts. Under simulated exhaust conditions (NO, CO, and N2O), Ru1/CeO2 enabled complete conversion of all three pollutants at 280 °C. Mechanistic studies revealed that N2O decomposition over Ru1/CeO2 and Run/CeO2 followed the Mars–van Krevelen (MvK) and Langmuir–Hinshelwood (L–H) mechanisms, respectively. The exceptional N2O decomposition activity of the single-atom catalyst stems from enhanced O2 desorption through the recombination of oxygen atoms that dissociate from N2O with adjacent lattice oxygen. Notably, Ru1/CeO2 exhibits remarkable O2 tolerance due to the selective adsorption: N2O binds to single Ru atoms, whereas O2 occupies oxygen vacancies. In contrast, the high energy barrier associated with O2 combination and desorption in Run/CeO2 hindered N2O decomposition, and the competitive adsorption of O2 on its surface led to poor O2 resistance. This study demonstrates Ru1/CeO2 as an efficient catalyst for abating N2O and multipollutant removal.
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PubMed
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 15
·e202501120
·
IF 2
Peipei Ji,Xiuwu Wang,Lianpei Zhou,Guiyang Zhou,Tao Chen
Graphical This study develops polymeric micelles with Brönsted acid and pybox-Ru(II) catalysts encapsulated in hydrophobic cores for efficient one-pot tandem catalysis of deacetalization-transfer hydrogenation. The micelles, prepared via self-assembly of block copolymers, demonstrate excellent catalytic efficiency, offering a simple and effective strategy for tandem catalysis. One-pot tandem catalysis has been favored by researchers for its ability to achieve the advantage of a shortened production process. In this paper, polymeric micelles containing Brönsted acid/pybox-Ru(II) in the hydrophobic cores were prepared for one-pot tandem catalysis of deacetalization-transfer hydrogenation reaction. First, block copolymer P[NHS] 30 - b -P[PEG 2000 ] 68 containing activated ester (NHS) in the suspended chain was successfully synthesized by ring-opening metathesis polymerization (ROMP) using a functional monomer containing norbornene group (NB-NHS) and polyethylene glycol containing norbornene group (NB-PEG 2000 ) as the raw materials. Then, block copolymer P[COOH] 30 - b -P[PEG 2000 ] 68 containing Brönsted acid catalyst and complex P[pybox-Ru] 30 - b -P[PEG 2000 ] 68 containing pybox-Ru(II) catalyst were prepared by the activated ester functionalization strategy. The copolymers and complexes were characterized using nuclear magnetic resonance spectroscopy (NMR), X-ray photoelectron spectroscopy (XPS), and gel permeation chromatography (GPC). Then, polymeric micelles with the catalysts encapsulated in hydrophobic cores were achieved by the self-assembly of the above copolymers in water. The prepared polymeric micelles as catalytic nanoreactors were successfully applied to one-pot tandem catalysis of the deacetalization-transfer hydrogenation reaction, demonstrating excellent catalytic efficiency. This study provided a facile and efficient strategy for tandem catalysis.
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Sustainability
·
2025
·Vol. 17
·期 10
·4358
·
IF 3.3
Yuantao Han,Yuchuan Ye,Wanjin Yu,Shaohong Zang,Lili Ji,Shijie Li,Liuye Mo
The synthesis of high performance catalysts for the catalytic wet oxidation (CWO) of N-methyldiethanolamine (MDEA) in water remains a challenge, and is a topic of considerable importance in relation to sustainability. In this paper, a Ru-CNx/CeO2catalyst was synthesized through a modified impregnation process for the CWO of MDEA, exhibiting a high activity of 80% COD removal at 180 °C and 2.5 MPa. EPR, Raman, and XPS characterizations revealed that the CNxspecies facilitated the reduction in Ru4+to Ru0species and enhanced the Ru–Ce interaction to form a high-density Ru-O-Ce structure with Ce3+sites, which strongly correlate to the generation of oxygen vacancies. The oxygen vacancies enabled the adsorption and activation of the oxygen, generating active species (h+, ·O2−, and ·OH) that effectively oxidized the MDEA during the catalytic reaction.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Yahui Ji,Nana You,Xiaoping Hu,Fei Wang,Gen Liu
The environmental hazards posed by bisphenol A (BPA) have become a critical global concern. Consequently, the development of rapid, user-friendly, and highly sensitive methods for BPA detection is essential for pollution control and health risk assessment. In this study, a novel electrochemiluminescent (ECL) sensor was designed using Ru(bpy) 3 2+ -encapsulated Zn-based metal–organic frameworks (Ru-ZnMOF) integrated with gold nanoparticles (Au@Ru-ZnMOF) as efficient ECL probes. Notably, BPA caused a significant quenching effect on the ECL signal of Au@Ru-ZnMOF in the presence of tripropylamine (TPA) as a coreactant. Under optimized experimental conditions, a glassy carbon electrode modified with Au@Ru-ZnMOF (glassy carbon electrode (GCE/Au@Ru-ZnMOF) demonstrated exceptional ECL performance for BPA detection, with a broad linear detection range (1.0 × 10 −9 to 5.0 × 10 −4 mol·L −1 ) and an ultra-low detection limit of 2.5 × 10 −11 mol·L −1 . The proposed sensor was successfully applied for the quantification of BPA in thermal paper samples, achieving recovery rates between 95.8 % and 98.5 %, confirming its high accuracy and reliability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Zihan Wei,Zhaonan Chong,Shujian Wang,Yan Chen,Run Cai,Change Yao,Zhong Ma,Guisheng Li
Ruthenium has regards as a potential electrocatalyst candidate towards hydrogen evolution reaction (HER) to substitute platinum and its surface property regulation is vital for increasing catalytic activity to realize the wide industrialization. Herein, we report a simple and facile method to regulate the metallic surface of Ru nanoparticles through high temperature calcination without particle overgrowth. The nanopores in Ketjenblack EC-600JD are employed as nanoreactors with Ru precursor ultrasonicated and impregnated and the subsize Ru nanoparticles embedded in porous carbon with highly metallic surface are obtained by high temperature annealing. The as-prepared Ru@KB-900 electrocatalyst shows excellent catalytic activity for HER with the overpotentials reached 9.9 mV and 28 mV at the current density of 10 mA cm −2 and the mass activities of 7404 A g Ru −1 and 478 A g Ru −1 at the overpotential of 50 mV, in acidic and alkaline electrolytes, respectively, which outperformed that of commercial Pt/C catalyst in the corresponding conditions. Furthermore, it also delivers a very good life-span performance at the overpotential of 50 mV over 48 h. The high HER activity is ascribed to the highly metallic surface of active site tuned by calcination temperature and the efficient exposure of active sites for the ultrasmall particle size. This study provides a simple and effective method for designing highly active sites with efficient exposure.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Longyang Liu,Zichen Wang,Xueyan Zhang,Lijie Luo,Yongjun Chen
Highly active and stable electrocatalysts are highly desired for the hydrogen evolution reaction (HER) in water electrolysis. In this study, a ruthenium-ruthenium phosphide heterojunction (Ru-Ru 2 P) anchored on phosphorus-doped graphene (PCSG) was fabricated via a mild molten salt template method. The graphene was synthesized from discarded coconut shells sourced from Hainan. We found that the heterojunction structure could accelerate electron transfer, while the graphene provided more exposed active sites, significantly enhancing the HER activity of the catalyst. The catalyst prepared at 800 °C with 30 mg of RuCl 3 (Ru-Ru 2 P/2D-PCSG-800) exhibited low HER overpotentials of 31 mV in alkaline and 57 mV in acidic electrolytes at a current density of 10 mA cm −2 , respectively, which were comparable to those of commercial 20 % Pt/C catalyst (36 mV in alkaline and 40 mV in acidic electrolytes). Moreover, the catalyst demonstrated high stability with no significant change in current density after 125 hours of operation. Density functional theory calculations revealed that the Ru-Ru 2 P heterojunction could rearrange charge and modify the Ru d -band center, optimizing the adsorption energy of active *H (|ΔG *H |) and breakage energy of *H-OH bond (ΔG H2O ).
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Advanced Science
·
2025
·
IF 14.1
Jie Li,Xue Wang,Jun Yu,Kai Xu,Zhe Jia,Hongkun Li,Lei Ren,Yiyuan Yang,Keke Chang,Yangyang Li,Xiangfa Liu,Jian Lu,Sida Liu
Development of active and cost-effective electrocatalysts to substitute platinum-based catalysts in alkaline hydrogen evolution reactions (HERs) remains a challenge. The synergistic effect between different elements in alloy catalysts can regulate electronic structure and thereby provide an abundance of catalytic sites for reactions. Thus, alloy catalysts are suitable candidates for future energy applications. Conventional methods for enhancing the performance of alloy catalysts have mainly focused on element composition and thus have often neglected to examine catalyst design. In this paper, a ruthenium–manganese–niobium alloy catalyst (Ru 62 Mn12Nb 21 O 5 ) is reported with a supra-nanocrystalline dual-phase structure that is fabricated through combinatorial magnetron co-sputtering at ambient temperatures. The induced crystal–crystal heterostructure of Ru 62 Mn 12 Nb 21 O 5 reduced system energy, thereby achieving balance between stability and catalytic activity. Ru 62 Mn 12 Nb 21 O 5 exhibited excellent HER performance, as demonstrated by low HER overpotential (18 mV at 10 mA cm −2 ) and robust stability (300 h at 1.2 A cm −2 ). Moreover, oxygen-rich interfaces in Ru 62 Mn 12 Nb 21 O 5 enhanced charge transfer and the kinetics of water dissociation as well as optimized hydrogen adsorption/desorption processes, thus boosting HER performance. The crystal–crystal heterostructure and oxygen-rich interfaces in Ru 62 Mn 12 Nb 21 O 5 are induced by its dual-phase nanocrystalline structure, which represents a new structural design for enhancing the performance of catalysts for sustainable energy development.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yang Shi,Pei Liu,Zhenluo Yuan,Xiaojiao Wang,Qiuming Peng,Shumin Han,Yanping Fan,Baozhong Liu
The exploitation of high-performance catalysts is essential for practical application of hydrogen production technology by ammonia borane (AB) hydrolysis. In this work, we reported an uncomplicated approach to exploit high-performance catalysts for hydrogen production from AB hydrolysis. Using the reducibility of AB, the Ru 0 /Mo 2 C MXene catalyst was synthesized using Mo 2 C MXene as carrier to hydrogen production from AB hydrolysis. The combination of Mo 2 C MXene and Ru nanoparticles exhibited remarkable catalytic performance. The TOF value was 868.6 min −1 and the hydrogen production rate reached as high as 210,464 mL min −1 g Ru −1 at 298 K. Moreover, the Ru 0 /Mo 2 C MXene catalyst showed good durability and continuously produce hydrogen for more than 4 h with a turnover number (TON) of 41293. Characterization analysis revealed that Mo 2 C MXene regulated the coordination environment of Ru, forming electron-rich Mo 2 C MXene and electron-deficient Ru sites. And excellent catalytic activity is benefiting from the enhanced interaction between Mo 2 C MXene and Ru nanoparticles, promoting the effective activation and dissociation of the reactants, which resulted in the improvement of the performance of AB hydrolysis. This work offers an innovative approach to synthesize efficient AB hydrolysis catalysts for hydrogen production.
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BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Chunyang Han,Zhen Dong,Yahui Zhang,Haian Xia
Ethylene glycol (EG) and 1,2-propylene glycol (1,2-PG) are very important chemicals that are produced mainly from fossil resources at present. Catalytic hydrogenolysis of biomass (such as cellulose and sugar alcohols) to diols has attracted much attention in recent years. However, compared to sugar alcohols, sugars such as xylose have been scarcely used for the production of EG and PG until now due to their instability and low selectivity of diols. Xylose is an abundant and readily available bio-chemicals that can be produced from the hydrolysis of hemicellulose, but its catalytic hydrogenolysis into diols with high yields remains a great challenge. Herein, bimetallic Ru-Re/CZO(Ce 0.7 Zr 0.3 O 2 ) catalysts were synthesized and used to catalyze the hydrogenolysis of xylose to EG and PG. The nature of the catalysts is thoroughly characterized by XRD, XPS, BET, TEM, etc. It is found that Ru and Re nanoparticles are uniformly distributed on CZO alloy support formed by Ce and Zr. A very high total yield (65.0 %) of EG and 1,2-PG was achieved on the 4 %Ru-1 %Re/CZO catalyst under optimal conditions. Recycling experiments demonstrate that high xylose conversion and diol yields are maintained over four successive cycles under optimal conditions, despite a slight increase in Ru nanoparticle size observed via TEM analysis. The mechanistic study shows that xylose is first isomerized into xylulose, which undergoes retro-aldol cleavage to generate the intermediates, followed by further hydrogenation to EG and 1,2-PG. This work provides a new research avenue for the efficient preparation of diols from xylose.
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Sustainable Materials and Technologies
·
2025
·
IF 9.2
Jingyuan Wei,Yanhui Song,Manyuan Gan,Guodong An,Yongqing Shen,Xiaohui Zhao,Yi Zhang,Peizhi Liu,Bingshe Xu,Junjie Guo
Modifying the catalyst's electronic structure is essential for improving the hydrazine oxidation reaction (HzOR) and alkaline hydrogen evolution reaction (HER), but it is still very difficult. We have developed a new heterostructured electrocatalyst in this work using Ru nanosheets and NiCo layered double hydroxides (LDH). In-situ Raman and theoretical studies show that the heterostructure of Ru/NiCo LDH lowers absorption of hydrogen's Gibbs free energy and the d-band center of Ru/NiCo LDH (from −1.7250 to −1.3341 eV), causing the directed development of interfacial H 2 O (ΔG H* , from 1.65 to 0.23 eV). With an overpotential of 19 and 75 mV to achieve 10 and 100 mA cm −2 for HER, these beneficial characteristics provide the Ru/NiCo LDH with exceptional electrocatalytic capabilities. For HzOR, 10 and 100 mA cm −2 may be produced using just −118 and−112 mV, respectively. The Ru/NiCo LDH electrolyzer also only needs 22 and 223 mV to produce 10 and 100 mA cm −2 , respectively. This work lays the groundwork for developing bifunctional catalysts for the green hydrogen industry.
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