ACS Catalysis
·
2022
·
IF 13.7
Yanliang Zhou,Xuanbei Peng,Tianhua Zhang,Hongfang Cai,Bingyu Lin,Lirong Zheng,Xiuyun Wang,Lilong Jiang
The metal–anion interaction (MAI) widely exists over supported metal catalysts, which has a significant effect on tuning metal sites and reaction performance. However, the effect of MAI on NH3 synthesis and the reaction mechanism is still elusive. Here, we report that the strength of Ru–anion interaction gradually increases from Ru–N to Ru–H and Ru–O when the anion of the support is changed from H (ZrH2) to N (ZrN) and O (ZrO2). Moreover, the Ru–anion interaction induced by different support compositions can affect the hydrogen spillover and N2 activation route. Due to the weak Ru–N interaction, the aggregation of Ru particles is observed over Ru/ZrN. Although Ru particles are highly dispersed over ZrO2 owing to the strong Ru–O interaction, hydrogen poisoning is inevitable over Ru/ZrO2. Comparatively, hydrogen poisoning can be alleviated over Ru/ZrH2 via hydrogen spillover to its support. The results of NEXAFS, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and isotope-labeling experiments show that N2 can be activated via both dissociative and associative routes over Ru/ZrH2. Consequently, the developed Ba-promoted Ru/ZrH2 catalyst displays a high NH3 synthesis rate of 27.5 mmol g–1 h–1 and robust stability during 300 h time-on-stream at 400 °C and 1 MPa.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Yaxi Gan,Ataollah Kalantari Osgouei,Alexander Ahrens,Bofang Wang,Jingyi Zhou,Jun-Zheng Zhan,Dan Zeng,Shengqiang Nie,Xinyuan Zhao,Guangxu Chen,Peter Nordlander,Linan Zhou
Plasmonic photocatalysis is promising for solar-driven chemical transformations under mild conditions; however, conventional materials like aluminum, copper, silver, and gold are resonant at short wavelengths, limiting their use in the red to near-infrared sunlight spectrum. In this study, we have developed a class of antenna-reactor (AR) photocatalyst based on two-dimensional (2D) plasmonic materials, Ti3C2Tx, also known as MXenes. A Ru-loaded Ti3C2Tx plasmonic photocatalyst achieves a turnover frequency of approximately 2 s–1 and energy efficiency of 10% for hydrogen production under 660 nm light excitation, being 2–3 orders of magnitude superior to the performance achieved in thermocatalysis. This 2D plasmonic antenna demonstrates superiority over the benchmark CuRu surface-alloy AR structure in hot-electron-driven processes under red light excitation. Kinetic studies suggest that the rate-determining step in both photo- and thermocatalysis is nitrogen’s associative desorption. Hot electrons enhance activity by promoting the removal of adsorbed nitrogenous species.
研究领域:
材料科学
·
化学工程
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DOI
PubMed
高影响因子
JOURNAL OF RARE EARTHS
·
2020
·
IF 3.104
Wei Li,Shuang Wang,Jinping Li
A series of BaCeO 3 modified with different rare earth elements (La, Y, Pr) were synthesized by co-precipitation and calcination and the effect of rare earth elements for catalytic ammonia synthesis under mild conditions was studied. The ammonia synthesis performance tests show that 2.5% Ru/BaCe 0.9 La 0.1 O 3– δ catalyst (All the percentages of Ru in this article are in mass fraction) exhibits the highest ammonia synthesis rate (34 mmol/(g·h)) at 3 MPa, 450 °C, and no sign of deactivation after 100 h of reaction. H 2 -TPR and XPS analyses indicate that the introduction of La increases the amount of oxygen vacancies of the catalyst, which is beneficial to increasing the electron density of Ru surface. HRTEM analysis shows that the Ru particle size is reduced greatly after La is introduced, which facilitates the catalyst generating more B 5 -type sites (active sites of Ru species for N N dissociation). CO 2 -TPD analysis indicates that BaCe 0.9 La 0.1 O 3– δ has stronger basicity , which promotes electrons transfer from support to Ru. This work provides an effective method for design and synthesis of Ru-based multi-element composite perovskite oxide catalysts.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Jingrong Li,Ying Wang,Tingting Xiao,Xinluona Su,Haiyang Cheng,Fengyu Zhao
Hydrogenation of aromatic molecules is a crucial industrial process that has been extensively employed in the synthesis of fundamental chemicals. In this work, the hydrogenation of bisphenol A (BPA) was studied over a kind of Ru/TiO2 catalyst. The catalytic activity of Ru/TiO2 was adjusted via manipulation of the metal–support interaction (MSI) by thermal treatment. The Ru/TiO2 exhibited a volcano-shaped dependence on calcination temperature, with the highest activity presented at 300 °C for the hydrogenation of BPA at mild conditions, produced 4,4′-isopropylidenedicyclohexanol (HBPA) with a yield of 99% at 80 °C, 4 MPa H2. The MSI could be adjusted by varying the calcination temperature, and flat Ru islands were formed at elevated temperatures, which facilitate the adsorption of the benzene ring of BPA. However, small-sized and electron-deficient Ru species prefer to adsorb H2. The Ru/TiO2-300 catalyst contains an appropriate composition of Ru nanoparticles and Ru flat islands, effectively balancing the competitive adsorption of H2 and BPA molecules, and thus exhibits high catalytic performance. Moreover, the Ru/TiO2-300 catalyst is highly efficient for a variety of aromatic compounds, producing the desired products selectively under mild conditions. Furthermore, it presented high stability without any loss in activity after 10 recycles. This work developed an efficient catalyst for the hydrogenation of aromatic compounds, and the insights into the catalytic mechanism will provide useful information to researchers in wide fields.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qinrui Sun,Ning Wang,Guihua Liu,Jingde Li,Xiaohang Du,Shujuan Sun
Dimensionally stable RuO 2 -based anodes have achieved excellent performance in the field of electrochemical treatment of wastewater, however, the high price of Ru hinders its industrial application. Herein, TiO 2 nanotubes-supported RuO 2 with ultralow Ru loading (0.34 wt%) and trace Fe and Mo doping (RuFeMo@TiO 2 ) was prepared as anode for efficient degradation of methylene blue. It shows that Fe and Mo doping reduce the oxidation state of Ru (Ru n+ , n < 4). In addition, the potential electroactive sites of the electrodes are effectively enhanced by Mo doping. While the Fe doping is found to improve the generation of hydroxyl radicals (·OH) and superoxide anion ( O 2 − ), which are the dominant oxidants for the degradation of methylene blue. In result, the RuFeMo@TiO 2 catalyst exhibits high performance towards methylene blue degradation of 97.5 % within 2 hours. It shows that the cooperation of trace transition metals enables efficient degradation of organic dye with ultralow-loaded Ru electrocatalyst, implying a promising application in wastewater treatment.
研究领域:
环境科学
·
电化学
·
废水处理
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Di Zhang,Jingjie Luo,Jiajie Wang,Xin Xiao,Yuefeng Liu,Wei Qi,Dang Sheng Su,Wei Chu
A series of Ru/FeO x catalysts were synthesized for the selective hydrogenation of CO 2 to CO. Detailed characterizations of the catalysts through X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and temperature-programmed techniques were performed to directly monitor the surface chemical properties and the catalytic performance to elucidate the reaction mechanism. Highly dispersed Ru species were observed on the surface of FeO x regardless of the initial Ru loading. Varying the Ru loading resulted in changes to the Ru coverage over the FeO x surface, which had a significant impact on the interaction between Ru and adsorbed H, and concomitantly, the H 2 activation capacity via the ability for H 2 dissociation. FeO x having 0.01% of Ru loading exhibited 100% selectivity toward CO resulting from the very strong interaction between Ru and adsorbed H, which limits the desorption of the activated H species and hinders over-reduction of CO to CH 4 . Further increasing the Ru loading of the catalysts to above 0.01% resulted in the adsorbed H to be easily dissociated, as a result of a weaker interaction with Ru, which allowed excessive CO reduction to produce CH 4 . Understanding how to selectively design the catalyst by tuning the initial loading of the active phase has broader implications on the design of supported metal catalysts toward preparing liquid fuels from CO 2 .
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Shaorong Deng,Chenji Zhu,Xiuzhong Fang,Xianglan Xu,Xiang Wang
A series of Ru-x%Li+/SiO2 catalysts (x = 0.05–0.2), modified with varying amounts of lithium cation (Li+), were prepared via coimpregnation and evaluated for CO2 methanation to explore Li+ modification on Ru/SiO2. Introducing trace Li+ markedly boosts reaction activity, with the optimal Ru-0.1%Li+/SiO2 exhibiting 38.4 and 12.3 times higher overall reaction rate and turnover frequency at 200 °C, respectively, compared to Ru/SiO2. Structural characterization confirmed that Li+ incorporation effectively suppresses RuO2 crystallization, thereby improving Ru dispersion from 9.1% to 31.5%, enhancing the active surface area from 33 to 115 m2 g–1, while simultaneously reducing Ru particle size from 18.4 to 3.2 nm. In situ spectroscopy and surface reaction experiments revealed that the CO* pathway occurs for CO2 methanation on both catalysts, which involves CO2 dissociation and subsequent CO* hydrogenation. The smaller Ru nanoparticles on Ru-0.1%Li+/SiO2 exhibit superior intrinsic activity for both steps compared to the larger nanoparticles on Ru/SiO2. The additional alkaline sites introduced by Li+ additives also promote CO2 dissociation. The exceptional activity of Ru-0.1%Li+/SiO2 for CO2 methanation is governed by the synergistic effect between the Ru particle size effect and Li+-induced basicity, with the former being predominant.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Yin Liu,Liang Shuai,Lei Cao,Qian Zhu,Lanlan Fan,Liang Xu,Shixian Xiong
The widespread use of carbendazim (CBZ) fungicide calls for monitoring its toxic residues in food due to human health concerns. Herein, a Ru/CeO 2-x heterostructured composite was constructed by sodium borohydride reduction for the electrochemical sensing of CBZ. The rational design engineers abundant interfacial oxygen vacancies and Ru nanoclusters, which form interfacial Lewis acid-base pairs capable of dual-site recognition of CBZ molecules. Specifically, oxygen-vacancy Lewis acidic sites preferentially adsorb the electron-rich groups(such as lone pairs on amino groups), while Ru-based Lewis basic sites capture electron-deficient carbon atoms within the benzimidazole ring. Such synergistic adsorption and interfacial charge transfer markedly enhance the redox kinetics of CBZ. Consequently, the Ru/CeO 2-x /GCE sensor delivers an ultralow detection limit of 7.7 nM, along with excellent selectivity, reproducibility, and long-term stability. This work provides a new interfacial engineering strategy integrating oxygen-defect chemistry and electronic modulation for designing high-performance Lewis acid–base coupled sensing materials.
研究领域:
环境监测
·
电分析化学
·
纳米材料
·
传感材料
·
食品安全
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产品关联
DOI
高影响因子
Communications Chemistry
·
2026
·
IF 6.9
Zhang Chengyu,Wang Longyu,Ndayisenga Fabrice,Jalil Anam,Zhang Yiming,Yu Zhisheng
The hydrogen evolution reaction (HER) is critical for clean energy conversion, yet achieving efficient and durable electrocatalysis across a wide pH range remains a major challenge. Modulating the electronic structure of metal single atoms has shown promise, but is often constrained by weak metal–support interactions in conventional carbon matrices. Here, we report a pH–universal HER electrocatalyst comprising atomically dispersed Ru sites and carbon–confined Ru nanoparticles, synthesized via one–step pyrolysis of biomass–derived precursors. The catalyst delivered low overpotentials of 176 mV (Tafel slope: 23 mV dec –1 ) in acidic and 241 mV (40 mV dec –1 ) in alkaline media at 200 mA cm –2 , along with outstanding operational stability exceeding 500 hours—outperforming commercial Pt/C. This performance arises from electron–rich Ru single atoms (RuN 4 ) modulated by neighboring Ru nanoparticles, synergistically embedded within a hydrophilic and porous carbon scaffold. Density functional theory (DFT) calculations revealed a near–optimal hydrogen adsorption free energy (ΔG H* = –0.25 eV) in acidic conditions and a moderate water dissociation barrier (0.94 eV) in alkaline media. Our findings demonstrate a viable strategy for integrating nanoparticles and single atoms to achieve both high activity and durability, while highlighting the upcycling of biomass into advanced HER catalysts via rational interface engineering.
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DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·1005-1016
·
IF 6.119
Qiang Zhou,Zijiang Zhao,Zihao Yao,Zhongzhe Wei,Songtao Huang,Fangjun Shao,Aiyuan Li,Jianguo Wang
Modulation of the metal–support interaction plays a key role in many important chemical reactions. Here, by adjusting the reduction method of the catalyst and introducing oxygen vacancies in TiO2 to regulate the interaction between Ru and TiO2, four supported Ru nanocatalysts with different encapsulation degrees and electronic structures were obtained. Ru nanoparticles (NPs) partially encapsulated by TiO2 can achieve the selective hydrogenation of 6-chloroquinoline even at room temperature, with a TOF of 12 h−1. Catalytic characterization and DFT calculations indicated that partially encapsulated Ru NPs not only provided active sites for H2 dissociation, but also reduced the probability of Ru NPs being poisoned. Meanwhile, the oxygen vacancies on the surface of TiO2 can adsorb 6-chloroquinoline molecules and provide additional active sites for hydrogenation via hydrogen spillover. Moreover, the enhanced electron transfer from oxygen-deficient TiO2 to Ru made Ru electron-rich, which repelled C–Cl bonds and effectively prevented the production of dechlorination products.
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DOI
高影响因子
Nano Energy
·
2020
·
IF 16.602
Ge Meng,Han Tian,Lingxin Peng,Zhonghua Ma,Yafeng Chen,Chang Chen,Ziwei Chang,Xiangzhi Cui,Jianlin Shi
Developing high-efficiency hydrogen evolution reaction (HER) catalysts is of great interest for the large-scale high-purity hydrogen production , which, unfortunately, is largely blocked by the sluggish kinetics of the electro-chemical dissociation step of water molecules. Herein, a MOF-derived method has been developed to prepare Ru nanoparticles-anchored sponge-like WNO embedded in N-doped carbon layers (Ru@WNO-C). The fabricated catalyst Ru@WNO-C (Ru: 0.9 wt%) shows excellent HER catalytic activity and long-term stability with the overpotentials of 172, 358 and 24 mV at 10 mA/cm 2 in 0.5 M H 2 SO 4 , 1 M Na 2 SO 4 and 1 M KOH, respectively. More impressively, the overpotentials, especially in neutral medium, decrease markedly during the durability tests owing to the catalyst structure activation after residual Zn species leaching. The enhanced catalytic activity of Ru@WNO-C during operation is mainly attributed to the in-situ electron donation from Ru to W, leading to the easier cleavage of highly polarized H‒OH bond of water molecules and thus endowing Ru@WNO-C with excellent HER catalytic performance in non-acidic solution.
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Luping Huang,Xinmeng Xu,Kun Wang,Wantao Zhang,Ziping Liu,Tianyu Qi,Feng Li,Qian Liu,Guiying Xu,Weimin Zhou
Oxygen-vacancy-rich TiO 2-x is uniformly coated on the surface of carbon black substrates. • Ru nanoparticles are highly dispersed on the TiO 2-x support. • TiO 2-x efficiently regulates the electronic structure of Ru sites, thus significantly boosting the electrocatalytic hydrogen evolution performance. The exploration of low cost, highly active, and stable catalysts for the hydrogen evolution reaction (HER) is the key to the future application of electrochemical water splitting. Herein, density functional theory (DFT) calculation results reveal that the oxygen vacancies TiO 2-x can effectively modulate the electron structure of Ru, thereby extremely enhancing the catalytic activity of Ru. Experimentally, to form an integrated nano-heterostructure, a facile approach is designed for the fabrication of super dispersed Ru nano particles on oxygen-deficient TiO 2-x , simultaneously combined with carbon black (CB) as a conductive network. Benefiting from the rich active sites, the optimized Ru/TiO 2-x /CB exhibited excellent catalytic performance, with overpotentials of 56 mV and 112 mV for the HER at a current density of 10 mA cm −2 in 1 M KOH and 0.5 M H 2 SO 4 , respectively. Ru/TiO 2-x /CB demonstrates superior stability and rapid HER kinetics under both acidic and alkaline conditions. Our studies provide a facile and feasible strategy for constructing high-performance water-splitting electrocatalysts. Download: Download high-res image (260KB) Download: Download full-size image
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