Nature Communications
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2024
·Vol. 15
·期 1
·1-9
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IF 14.7
Chen Min,Liu Longgang,Chen Xueyan,Qin Xiaoxiao,Zhang Jianghao,Xie Shaohua,Liu Fudong,He Hong,Zhang Changbin
Efficient heterogeneous catalyst design primarily focuses on engineering the active sites or supports, often neglecting the impact of trace impurities on catalytic performance. Herein, we demonstrate that even trace amounts of sulfate (SO 4 2− ) residuals on Ru/TiO 2 can totally change the CO 2 reduction from methanation to reverse-water gas shift (RWGS) reaction under atmospheric pressure. We reveal that air annealing causes the trace amount of SO 4 2− to migrate from TiO 2 to Ru/TiO 2 interface, leading to the significant changes in product selectivity from CH 4 to CO. Detailed characterizations and DFT calculations show that the sulfate at Ru/TiO 2 interface notably enhances the H transfer from Ru particles to the TiO 2 support, weakening the CO intermediate activation on Ru particles and inhibiting the further hydrogenation of CO to CH 4 . This discovery highlights the vital role of trace impurities in CO 2 hydrogenation reaction, and also provides broad implications for the design and development of more efficient and selective heterogeneous catalysts.
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Materials Today Communications
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2024
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IF 3.7
Cheng Chen,Jingbao Zhang,Lihua Zhu,Yu Fang,Jinhui Li,Huan Zhang
The Ru/WO 3 catalysts with various Ru contents (Ru weight percent-0.47 %, 0.96 %, 1.91 %, denoted as Ru/WO 3 -1, 2, 3, respectively) are prepared through NaBH 4 liquid phase chemical reduction strategy. Ru is uniformly dispersed as nanoparticles and nanoclusters on the WO 3 nanorods, and the catalytic performance of the Ru/WO 3 -3 catalysts for furfural (FF) selective hydrogenation at relatively mild conditions (reaction temperature-60 ℃, reaction time-8 h, hydrogen pressure-2.0 MPa) is investigated. It is found that the Ru/WO 3 -3 catalyst exhibits the most excellent catalytic performance, with 85.2 % conversion of FF, 97.3 % selectivity of furfuryl alcohol (FA), and highly stable. Characterization of XRD, XPS, TEM, HRTEM, H 2 -TPD, H 2 -TPR, N 2 -physical adsorption-desorption, STEM-EDX elemental line-scannig and mapping reveal that there is a synergistic effect and strong interaction between Ru and WO 3 . The ruthenium nanoclusters and nanoparticles are beneficial to the activation of H 2 , forming activated hydrogen species (H*), the interface of Ru-O-W is in favor of the adsorption and activation of C O, thus improving the selectivity of C O hydrogenation and forming FA.
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Energy Storage Materials
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2022
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IF 20.831
Xuecheng Cao,Chaohui Wei,Xiangjun Zheng,Kai Zeng,Xin Chen,Mark H. Rummeli,Peter Strasser,Ruizhi Yang
Lithium–oxygen (Li–O 2 ) batteries have attracted tremendous attention due to their high specific energy density . However, their sluggish conversion kinetics and detrimental parasitic reactions would deteriorate the lifespan of batteries. Herein, a combined density functional theory (DFT) calculation and experimental approach is carried out to design an efficient cathode electrocatalyst for Li–O 2 batteries. A self-supporting film of Ru clusters anchored on Magnéli phase Ti 4 O 7 enriched with oxygen vacancy (Ru/Ti 4 O 7 ) is fabricated upon electrospinning and carbothermal reduction. In such a synergistic configuration of Ru/Ti 4 O 7 hybrid film, the strong metal-support interaction (SMSI) between Ru and Ti 4 O 7 can improve the charge transfer at the interface and enhance the adsorption energy of intermediates, accelerating the reaction kinetics of the formation/decomposition of Li 2 O 2 . Benefitting from this SMSI, the electrochemical stability of Ru/Ti 4 O 7 over cycling is also enhanced. As a result, as-prepared Ru/Ti 4 O 7 cathodes could realize excellent electrochemical performance , including high specific capacity (11000 mAh g –1 ), low discharge/charge polarization (0.36 V), long lifespan (> 100 cycles) and superior rate capability. Furthermore, a flexible Li–O 2 pouch cell, constructed with as-fabricated Ru/Ti 4 O 7 film cathode, lithium foil anode and GPE , can exert an impressive areal capacity of 5 mAh cm –2 with a low voltage gap of 0.82 V in ambient air. This work suggests that the activity of catalysts can be significantly enhanced with interfacial modification, offering an efficient approach for rational designing of electrocatalysts for use in Li–air batteries and beyond.
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CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Xuanbei Peng,Yongjin Luo,Tianhua Zhang,Jinxiu Deng,Yanliang Zhou,Jiaxin Li,Jun Ni,Bingyu Lin,Jianxin Lin,Dongshuang Wu,Lirong Zheng,Xiuyun Wang,Lilong Jiang
The effects of promoters on Ru nanoparticles (≥2 nm) catalysts for NH 3 synthesis have been extensively elaborated, but their roles on ultrasmall Ru nanoclusters (NCs, 1–2 nm) remain largely unknown and need to be further uncovered. Herein, a series of K-promoted MgO supported Ru NCs were synthesized and investigated for NH 3 synthesis. The addition of 5wt.%K onto Ru/MgO NCs leads to a significantly high NH 3 synthesis rate of 21.7 mmol NH3 g cat −1 h −1 at 400 °C and 0.2 MPa, close to the thermodynamic equilibrium. Out studies reveal that anchoring K onto Ru NCs can increase the electron density and cause an upshift of the d -band center of Ru entities. Moreover, the addition of K regulates the hydrogen affinity and accelerates the migration of hydrogen from the Ru NCs surface to MgO support, which is crucial in avoiding the hydrogen poisoning effect on Ru NCs. With the synergistic effect of the Ru NCs sites bridged by H-spillover, makes the K-mediated Ru/MgO NCs catalysts efficient for NH 3 synthesis at mild conditions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Kunjie Wang,Xianrong Liu,Yanan Li,Yunsi Wang,Riming Hu,Bingxin Liu,Peng Zhang,Benhua Xu,Yongcheng Li
Ensuring Ruthenium-based (Ru) catalysts with high metal utilization is a potential and challenging strategy for designing and constructing high catalytic activity electrocatalysts for hydrogen evolution reaction (HER). Herein, Ruthenium single atoms (SA) and Ruthenium nanoparticles (NPs) are simultaneously anchored on hierarchically porous carbon via the self-templates method for the first time. Benefiting from the synergetic effect of hierarchically porous carbon and the coexistence of Ru SA and Ru NPs, the Ru/C-800 shows attractive HER catalytic activity in acidic and alkaline solutions, with low overpotentials to drive the current density of 10 mA cm −2 and the smallest Tafel slope. Density functional theory (DFT) results reveal that the coexistence of Ru SA and Ru NPs can positively affect charge distribution and charge transfer kinetics, and reduce the hydrogen adsorption and water dissociation free energy. This work provides a novel self-templating strategy for synthesizing high catalytic activity catalysts in a wide pH range.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Jinjing Qiu,Qi Chen,Cheng Liu,Yueling Chen,Jionghua Wu,Kaiqiang Jing,Jimmy C. Yu,Ling Wu,Xianzhi Fu
Defect engineering and single atom incorporation can provide more active sites to modulate the surface electronic structure of a catalyst and to activate reactant molecules. Herein, a series of Ru-anchored DUT-67(Zr) MOFs with explicit defect sites have been prepared for photocatalytic nitrogen reduction. It is characterized that Ru/DUT-67(Zr) possesses uniformly dispersed Ru single atoms and unsaturated Zr. Typically, 1.0 %Ru/DUT-67(Zr) shows best performance with a NH 4 + yield of 61.1 μmol·g −1 ·h −1 , which is approximately 6-folds higher than that of defective DUT-67(Zr) without Ru single atom (DUT-L), while pristine DUT-67(Zr) exhibits a lack of the photocatalytic N 2 reduction activity. The observed enhancement can be attributed to the introduction of Ru and unsaturated Zr sites induced by irradiation. Both of them can work together act as active centers to absorb and activate dinitrogen molecule. Furthermore, benefited from the electronic channel (Ru-S) between Ru and DUT-67(Zr), the separation of photogenerated carriers has been greatly improved, contributing to the collaborative conversion of activated N 2 to NH 3 . This study provides a new insight for designing a dual active sites photocatalyst with unsaturated coordinated sites and the single atoms by the coordinately interaction of functionalized linker.
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INORGANIC CHEMISTRY
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2024
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IF 4.3
Huijiao Wang,Gening Du,Jinzhi Jia,Junfeng Huang,Mudong Tu,Jinhua Zhang,Yong Peng,Hua Li,Cailing Xu
The Electrochemical reduction of nitrate to ammonia (NH3) is a process of great significance to energy utilization and environmental protection. However, it suffers from sluggish multielectron/proton-involved steps involving coupling reactions between different reaction intermediates and active hydrogen species (Hads) produced by water decomposition. In this study, a Ru-doped NiFe-MIL-53 (NiFeRu-MIL-53) supported on Ni foam (NF) has been designed for the nitrate reduction reaction (NO3RR). The NiFeRu-MIL-53 exhibits excellent NO3RR activity with a maximum Faradaic efficiency (FE) of 100% at −0.4 V vs. RHE for NH3 and a maximum NH3 yield of 62.39 mg h–1 cm–2 at −0.7 V vs. RHE in alkaline media. This excellent performance for the NO3RR is attributed to a strong synergistic effect between Ru and reconstructed NiFe(OH)2. Additionally, the doped Ru facilitates water dissociation, leading to an appropriate supply of Hads required for N species hydrogenation during NO3RR, thereby further enhancing its performance. Furthermore, in situ Raman analysis reveals that incorporating Ru facilitates the reconstruction of MOFs and promotes the formation of hydroxide active species during the NO3RR process. This work provides a valuable strategy for designing electrocatalysts to improve the efficiency of the reduction of electrochemical nitrate to ammonia.
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RENEWABLE ENERGY
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2025
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IF 9.1
Yongyuan Deng,Yichao Ye,Tao Yin,Zhipeng Tian,Chao Wang,Ying Chen,Zhi Yang,Junling Tu,Riyang Shu
Hydrodeoxygenation (HDO) is a common refinery process to convert oxygen-containing lignin pyrolysis oil into high-quality hydrocarbon liquid fuels. In this work, we prepared a core-shell Ru@SiO 2 -Al 2 O 3 catalyst and employed it in the HDO of phenolic compounds and lignin pyrolysis oil. The unique core-shell structure of the catalyst reduces the size of Ru metal particles, which significantly improves the hydrogenation catalytic activity. The high surface area, large pore size, and large pore volume of the SiO 2 shell provide a favorable environment for the substrate transfer during the reactions, meanwhile the doped Al 2 O 3 introduces a substantial number of acid sites for the catalysis of deoxygenation. The synergistic effect between the metal sites and acid sites greatly promotes the HDO reaction efficiency. Under mild conditions of 220 °C and 1 MPa H 2 , Ru@SiO 2 -Al 2 O 3 catalyst achieved a guaiacol conversion of 99.9% and a cyclohexane selectivity of 99.9%. This catalyst also demonstrates an outstanding stability, with catalytic activity little loss after 6 recycles. Furthermore, an efficient HDO performance was obtained in the upgrade of other phenolic compounds and lignin pyrolysis oil. At the temperature of 240 °C, the content of hydrocarbons in lignin pyrolysis oil increased from 15.4% to 92.7%. These results indicate that Ru@SiO 2 -Al 2 O 3 holds significant potential for the efficient HDO refinery, providing a promising avenue for the future biofuel development.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Jingwei Du,Jinjun Li,Zhixiong You
This study explores the preparation of a Cs-doped Ru/ZrO 2 catalyst using a low eutectic system and its application in ammonia synthesis. Additionally, it examines the effect of Cs doping on enhancing the catalyst's resistance to hydrogen poisoning. Compared to the undoped Ru/ZrO 2 catalyst and the Cs–Ru/ZrO 2 –B catalyst prepared through the grinding method for promoter incorporation, the Cs–Ru/ZrO 2 -A catalyst synthesized using the low eutectic system demonstrated significantly enhanced activity. At 400 °C and 0.1 MPa, the Cs–Ru/ZrO 2 -A catalyst achieved an ammonia synthesis activity of 1769 μmol g cat −1 h −1 , which is approximately 35 times higher than that of the undoped Ru/ZrO 2 catalyst. The structure of the catalyst was analyzed using various material characterization techniques, including XRD, XPS, and SEM. The results showed that the Cs–Ru/ZrO 2 -A catalyst, prepared under identical conditions, exhibited no significant structural differences compared to other catalysts. However, further TPR and TPD analyses revealed that Cs interacts with Ru to some extent, affecting its reduction behavior and enhancing the catalytic reaction rate for ammonia synthesis. Additionally, detailed XPS analysis of all catalysts was conducted, leading to a proposed relationship between the catalytic reaction rate and the oxidation states of the metal components. The study revealed that the presence of Cs significantly inhibits hydrogen poisoning of the catalyst. Furthermore, it demonstrated that the addition of promoters enhances H 2 dissociation by supplying electrons to the active metal Ru, while Cs plays a crucial role in effectively suppressing hydrogen poisoning.
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MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 5
·1-11
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IF 5.3
Tian Li,Li Huiling,Han Pengfei,Ma Guangping,Wang Wenzhuo,Jiang Hanyue,Lu Juan
An electrochemiluminescence (ECL) sensor was constructed based on Ru(bpy) 3 2+ @Au and GO@CdS for the detection of tartrazine (TTZ). In the presence of the co-reactant TPrA, Ru(bpy) 3 2+ and CdS quantum dots (QDs) were used as dual luminophores to synergistically amplify the ECL signal of the sensor. Gold nanoparticles (Au NPs) enhanced the electron transport capability of the system and thereby amplified the ECL intensity. Graphene oxide (GO), as a carrier, has a special wrinkle-like structure that not only adsorbed a substantial amount of CdS QDs but also prevented their agglomeration. Additionally, a more sensitive detection method was established based on the quenching of the ECL signal, which occurred due to the interaction between Ru(bpy) 3 2+ and TTZ. A low detection limit (1.3 × 10 –13 mol·L −1 , S/N = 3) was obtained for TTZ concentrations ranging from 4.0 × 10 –13 to 4.0 × 10 –8 mol·L −1 . Finally, actual measurement results from three beverage samples demonstrated that the prepared sensors possess excellent practical capabilities for TTZ detection. Graphical
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Hairui Cai,Nan Jiang,Laifei Xiong,Fanfan Shang,Yuyan Tang,Xiaojing Zhang,Chenyu Liang,Di Su,Shengchun Yang
Ruthenium, a promising lower-cost, high-activity alternative to iridium for acidic PEMWE oxygen evolution, requires innovative stabilization and bifunctionality enhancement strategies due to its dissolution and nanoparticle instability under OER conditions and inferior HER activity compared to platinum. Herein, a novel strategy for bifunctional acidic water electrolysis catalysts integrates Y-doped Ru nanoparticles onto CNT-decorated carbon cloth (Y–Ru/CNT/CC), yielding high activity and stability. Introducing Y atom shifts the Ru d-band center negatively, reducing excessive adsorption of oxygen-containing intermediates and improving OER stability, while optimizing the hydrogen adsorption free energy (ΔGH*) for enhanced HER activity. Furthermore, the CNT support provides a highly conductive network and abundant anchoring sites, which cooperate with Y-doping to inhibit Ru dissolution migration under acidic conditions. The catalyst exhibited excellent bifunctional activity in 0.5 M H2SO4 (HER: η10 = 27 mV; OER: η10 = 185 mV), which was significantly better than that of commercial Pt/C and RuO2. This study presents a novel approach to designing a cost-effective acidic electrolytic water catalyst, promoting the practical application of PEMWE technology.
研究领域:
电催化
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材料科学
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可再生能源
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纳米材料
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水分解
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Xiaolong Tan,Xiangguo Zhang,Yushi He,Zeyi Jiang,Cheng Bao,Nien-Chu Lai
Carbon monoxide selective methanation (CO-SMET) holds promise for removing low-concentration CO in the hydrocarbon reforming for hydrogen (H 2 ) production process and is a deep CO removal technology suitable for low-temperature fuel cells. However, developing highly efficient CO-SMET catalysts remains a significant challenge. Herein, we report a supported catalyst (Ru 1.0 (Cl)/TiO 2 ) with highly dispersed ruthenium (Ru) metal on a high-specific-surface-area mesoporous titanium dioxide (TiO 2 ) catalyst. This catalyst exhibits excellent performance in CO-SMET. It can reduce the CO concentration to below 10 ppm in a wide temperature range of 190–300 °C, and the outlet CO concentration can reach an ultra-low level of 0.2 ppm in the optimal temperature zone (210–220 °C). Through XPS and in situ DRIFTS characterizations, the crucial role of Ru–Cl species at the metal-support interface is revealed. The presence of chlorine atoms leads to electron enrichment in the Ru metal, enhancing its adsorption and activation of CO.
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