TALANTA
·
2025
·
IF 6.1
Tingting Wang,Xinhua Zhao,Zhenxu Li,Yi Zhang,Zhu Zhang,Dachi Yang
The newly-emerged gas sensing detection of 1-octen-3-ol biomarker is expected to indirectly monitor foodborne illnesses caused by Salmonella-contaminated meat, which requires high selectivity and a ppb-concentration detection limit. Here, surface-doped ruthenium over tungsten oxide nanocubes (Ru/WO 3 NCBs) have been synthesized by a wet-chemical approach for highly selective and ppb-concentration 1-octen-3-ol sensing. As-prepared Ru/WO 3 NCBs exhibit a polycrystalline structure and consist of NCBs that have an average side length of ∼131 nm, and the Ru/WO 3 NCBs show a high sensing response toward 5 ppm 1-octen-3-ol (R a /R g = 406), excellent selectivity, 50 ppb detection limit, 70% relative humidity tolerance, and 54 days stability at 220 o C. The excellent sensing performance might be attributed to the electronic and chemical sensitization of Ru, which thickens the electron depletion layer and increases adsorbed oxygen to promote interfacial electron transfer and 1-octen-3-ol oxidation. Practically, Ru/WO 3 NCBs have been integrated into a sensing device to simulate detecting 1-octen-3-ol, which has the potential for Salmonella detection in the future.
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GREEN CHEMISTRY
·
2025
·
IF 9.2
Liwu Qiang,Meng Bai,Zonghang Liu,Peipei Zhao,Shuai He,Man Zhao,Qinyun Yan,Wei Wen,Qilin Guo,Yanxia Zhang,He Xiao,Jianfeng Jia
The development of efficient pH-universal electrocatalysts for the hydrogen evolution reaction (HER) remains a critical challenge in renewable energy technologies. While Pt-based catalysts exhibit exceptional activity in acidic media, their performance deteriorates significantly in alkaline and neutral conditions due to sluggish water dissociation kinetics. Here, a carbon dots (CDs)-driven strategy is designed to engineer the spatial distribution and electronic structure of Ru species on graphene, achieving remarkable HER activity across the full pH range. By modulating the Ru-CDs interfacial configuration from CDs@Ru-coated to Ru&CDs-dispersed and Ru@CDs-encapsulated structures, it’s found Ru-6CDs/G exhibits excellent performance with the planar Ru&CDs arrangement. This Ru-6CDs/G catalyst exhibits ultralow overpotentials of 77 mV (0.5 M H₂SO₄), 58 mV (1.0 M KOH), and 39 mV (0.5 M PBS) at 10 mA cm-², alongside exceptional mass activities surpassing commercial Pt/C by up to 129 times. Combined experimental and theoretical analyses reveal that the Ru&CD configuration with optimal dispersion and the smallest size (~1.14 nm) of Ru nanoparticle induces a moderate d-band center position, balancing hydrogen adsorption/desorption energetics and accelerating the Volmer-Heyrovsky pathway. Density functional theory (DFT) calculations further demonstrate that charge redistribution at the Ru-CDs interface enhances H* intermediate stabilization, while COHP analysis confirms optimized Ru-H bond strength. This work not only establishes a universal design principle for metal-CDs hybrid catalysts but also provides deep insights into the electronic and spatial regulation of active sites for advanced electrocatalysis.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yanling Wang,Lishi Luo,Tuotuo Zhang,Jun-Rui Hu,Huiling Wang,Feng Bao,Chonglu Li,Yao Sun,Junrong Li
Sonodynamic therapy (SDT) can generate reactive oxygen species (ROS) to combat multidrug-resistant biofilms, which pose significant challenges to human health. As the key to producing ROS in SDT, the design of sonosensitizers with optimal molecular structures for sufficient ROS generation and activity in complex biofilm matrix is essential. In this study, we propose a π-expansion strategy and synthesize a series of small-molecule metal Ru(II) complexes (Ru1–Ru4) as sonosensitizers (Ru1–Ru4) to enhance the efficacy of SDT. Among these complexes, Ru4 demonstrates remarkable ROS generation capability (∼65.5-fold) that surpasses most commercial sonosensitizers (1.3- to 6.7-fold). Through catalyzing endogenous H2O2 decomposition, Ru4 facilitates the production of abundant O2 as a resource for 1O2 and the generation of new ROS (i.e., •OH) for improving SDT. Furthermore, Ru4 maintains the sustained ROS activity via consuming the interferences (e.g., glutathione) that react with ROS. Due to these unique advantages, Ru4 exhibits potent biofilm eradication ability against methicillin-resistant Staphylococcus aureus (MRSA) both in vitro and in vivo, underscoring its potential use in clinical settings. This work introduces a new approach for designing effective sonosensitizers to eliminate biofilm infections, addressing a critical need in healthcare management.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Ruofan Shen,Yanyan Liu,Hao Wen,Tao Liu,Zhikun Peng,Xianli Wu,Xianghong Ge,Sehrish Mehdi,Huaqiang Cao,Erjun Liang,Jianchun Jiang,Baojun Li
High activity catalysts used for eliminating the energy barrier in water breaking-up are of great significance for accelerating those reactions retarded by water molecules dissociation. In this work, an oxygen vacancy (V O )-Ti ensemble engineering on Ru catalyst was established to boost the catalytic activity toward water dissociation. The V O in V O -Ti ensemble plays as electron promoter to transfers electrons to surface Ru atoms. The rich electron state of Ru boosts the catalytic activity toward water dissociation. As an experimental verification, the turnover frequency of 1.5-RTV O -4 in ammonia borane hydrolysis reaches up to 1370 min −1 (9710 min −1 depend on the dispersion of Ru), exceeding the benchmark value set up by Ru-based catalysts. This research provides a novel electronic tuning strategy for V O as imaginary atom via electron promoter effect to enhance the intrinsic catalytic activity of metal catalysts toward inert molecule dissociation in the next generation energy chemistry field.
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Chem
·
2021
·
IF 22.804
Lingling Li,Ya-Fei Jiang,Tianhua Zhang,Hongfang Cai,Yanliang Zhou,Bingyu Lin,Xingyi Lin,Ying Zheng,Lirong Zheng,Xiuyun Wang,Cong-Qiao Xu,Chak-tong Au,Lilong Jiang,Jun Li
Summary Ammonia synthesis is structure sensitive, and a minute change in the catalyst structure would cause a dramatic change in activity. To date, none of the studies reveal the metal size effect at a subnanometer scale on NH 3 synthesis, and such investigation remains a challenge. Here, we report the synthesis of Ru catalysts with sizes ranging from single atoms, atomic clusters (ACCs), sub-nanometric clusters, to nanoparticles (NPs) by adjusting precursor and/or loading of Ru. Sub-nanometric Ru catalysts not only exhibit performance different from that of NPs but also follow a different route for N 2 activation. The strong intra-cluster interaction of Ru atomic clusters enables the formation of strong interactions of Ru d -orbitals with the σ and π orbitals of N 2 molecules, resulting in N 2 activation over Ru ACCs to occur more easily than that over Ru NPs. Consequently, Ru ACCs display an unprecedentedly high NH 3 synthesis rate and large turnover frequency at mild conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Wenkang Xu,Xiaoyao Li,Chao Peng,Guangxing Yang,Yonghai Cao,Hongjuan Wang,Feng Peng,Hao Yu
MXenes, 2D transition metal carbides/nitrides, have been demonstrated as promising platform for fabricating novel composites with interesting photo-/electrochemical properties. It is desirable to gain insights into the reactivity of MXenes, enabling the controllable transformation of MXenes. Here, a one-pot hydrothermal synthesis method of MXene-based photocatalyst is validated by harnessing the reducibility of Nb 2 CT x MXene . The origin of reducibility of Nb 2 CT x during the hydrothermal oxidation process was demonstrated as the active hydrogen produced from the water splitting in the presence of Nb 2 CT x , which reduced Ru 3+ in situ to Ru nanoparticles on Nb 2 O 5 nanowires derived from Nb 2 CT x . Compared with the traditional photo-deposition method, the chemical valance of the noble metal Ru/Pt obtained by the one-pot synthesis method was closer to the metal state, which reduced the charge transfer resistance by 82.5%. It led to the photocatalytic hydrogen production of 10.11 mmol·h −1 ·g −1 with 41.25% apparent quantum yield at 313 nm.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Shu-Hu Yin,Xiao-Yang Cheng,Yu Han,Ting Zhu,Zhong-Wei Yu,Rui Huang,Jun Xu,Yan-Xia Jiang,Shi-Gang Sun
Fe-N-C catalysts are promising substitutes for precious-metal platinum in acidic oxygen reduction reactions (ORR), yet their moderate intrinsic activity and susceptibility to reactive oxygen species (ROS)-induced degradation hinder practical implementation. Herein, we fabricate a Ru-Fe dual-site catalyst (RuFe-N-C) through a two-step pyrolysis strategy. Structural characterization reveals atomic-scale proximity between Ru single atoms and Fe-N 4 moieties, exhibiting a projected distance of ~1.7 Å. This configuration induces Fe–N bond elongation accompanied by 2.5% lattice distortion. The optimized RuFe-N-C catalyst exhibits high ORR performance, with a half-wave potential ( E 1/2 ) of 0.840 V and peak power density ( P max ) of 938 mW cm –2 under 150 kPa absolute H 2 -O 2 . These metrics signify substantial enhancements relative to conventional Fe-N-C benchmarks (+21 mV in E 1/2 and +42% in P max ). Moreover, the catalyst maintains outstanding stability, showing merely 17 mV E 1/2 decay after 10000 accelerated durability test (ADT) cycles. Experimental analyses reveal a bifunctional mechanism: (1) Adjacent Ru sites substantially enhance the intrinsic ORR activity of Fe-N 4 moieties, delivering a notable turnover frequency (TOF = 17.86 e site –1 s –1 at 0.85 V vs. RHE) that exceeds state-of-the-art Fe-N-C benchmarks by 1–2 orders of magnitude (< 1 e site –1 s –1 ); (2) Ru centers function as electron relays that facilitate ROS scavenging, thus suppressing degradation. This work establishes a paradigm for engineering bimetallic single-atom catalysts through synergistic electronic modulation to concurrently enhance activity and stability.
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Matter
·
2024
·
IF 17.3
Lingfeng Li,Jiaming Zhu,Fanpeng Kong,Yijie Wang,Cong Kang,Ming Xu,Chunyu Du,Geping Yin
Elucidating how the local strain environment of single atoms affects their impact on a sluggish acidic oxygen reduction reaction (ORR) is important for the design and construction of highly active electrocatalysts. Here, we report that the atomic strain geometry of Fe single sites is exclusively regulated by the communicative effects of dual atoms. Theoretical analysis reveals that Fe-Ru dual atoms in a moderate strain environment achieve the lowest Gibbs free energy barrier during an ORR. Impressively, FeRu-N-C with an FeRuN 8 moiety exhibits the highest acidic ORR performance, with a half-wave potential ( E 1/2 ) of 0.860 V and only a 17-mV loss in E 1/2 after 50,000 potential cycles. Operando characterization and electronic configuration analysis demonstrate that moderately strained Fe sites promote hydrogenation desorption of (oxy-)hydroxyl by enabling more electrons to occupy antibonding orbitals. This study describes a promising way of investigating high-performance single-atom-based catalysts by tailoring the atomic strain environment.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Zhao Jia,Urrego-Ortiz Ricardo,Liao Nan,Calle-Vallejo Federico,Luo Jingshan
Electrocatalysis holds the key to enhancing the efficiency and cost-effectiveness of water splitting devices, thereby contributing to the advancement of hydrogen as a clean, sustainable energy carrier. This study focuses on the rational design of Ru nanoparticle catalysts supported on TiN (Ru NPs/TiN) for the hydrogen evolution reaction in alkaline conditions. The as designed catalysts exhibit a high mass activity of 20 A mg −1 Ru at an overpotential of 63 mV and long-term stability, surpassing the present benchmarks for commercial electrolyzers. Structural analysis highlights the effective modification of the Ru nanoparticle properties by the TiN substrate, while density functional theory calculations indicate strong adhesion of Ru particles to TiN substrates and advantageous modulation of hydrogen adsorption energies via particle-support interactions. Finally, we assemble an anion exchange membrane electrolyzer using the Ru NPs/TiN as the hydrogen evolution reaction catalyst, which operates at 5 A cm −2 for more than 1000 h with negligible degradation, exceeding the performance requirements for commercial electrolyzers. Our findings contribute to the design of efficient catalysts for water splitting by exploiting particle-support interactions.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yue Yu,Feng Liu,Xuanzhi Liu,Longquan Li,Binhua Zhou,Hanxiao Liao,Pengfei Tan,Jun Pan
The inevitable electrochemical oxidation accompanied with continuous dissolution of Ru triggers structural distortion, causing insufficient catalytic activity and stability of Ru-based electrocatalysts in acidic oxygen evolution reaction (OER). In this work, we propose a Mn doping strategy to obtain Mn doped RuO 2 (Mn-RuO 2 ) for stabilizing the dynamic Ru. X-ray absorption spectroscopy and X-ray photoelectron spectroscopy results indicate that the doped Mn in RuO 2 preferentially replaces the oxidation of Ru by self-oxidation during the OER process, which significantly suppresses excessive dissolution of Ru. Furthermore, in-situ Raman spectroscopy, in-situ electrochemical impedance spectroscopy, the differential electrochemical mass spectrometry measurements combined with density functional theory calculations demonstrate that the Mn doping is able to strengthen the covalency of metal–oxygen bonds, facilitate lattice oxygen mechanism with elevated energy level of O 2p band. Therefore, Mn-RuO 2 catalyst demonstrates remarkable acidic OER performance, only needing an overpotential of 209 mV to achieve the current density of 10 mA cm –2 , 139 mV lower than that of commercial RuO 2 . And Mn-RuO 2 can maintain stable operation for over 180 h, which is about 18 times that of commercial RuO 2 . Notably, when Mn-RuO 2 is used as the anode, the proton exchange membrane water electrolyzers demonstrates stable operation for 40 h at 100 mA cm −2 . This work offers a strategy to alleviate stability issue of Ru-based catalysts for efficient acidic OER process.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xitong Yang,Guowei Liu,Ruifeng Zhou,Zhengzheng Xie,Yamin Cheng,Muhammad Shuaib Khan,Qiuye Li
Catalytic desorption can reduce the activation energy of the reaction and increase the desorption reaction rate, and is one of the most promising technologies to solve energy consumption problems of CO 2 capture technology for organic amine solutions. In order to further reduce desorption energy consumption, we propose a new method of utilizing the photothermal effect of catalysts to increase desorption temperature and accelerate reaction kinetics, and coupling the proton transfer ability of the catalyst itself to form multifunctional catalysis. In this work, we synthesized Ru x Mn 1-x OOH catalyst by introducing Ru atoms at the Mn vacancies on the MnOOH surface, grasping the advantages of the photothermal and proton transfer ability of Ru-dopants. The results showed that the CO 2 desorption capacity increased by 43.1% with adding MnOOH compared to without a catalyst. The Ru-doped catalyst demonstrated a 54.7% increase in CO 2 desorption efficiency, with an additional 98.2% surge attributed to the in-situ photothermal effect generated by the catalyst under light irradiation. Characterization and density functional theory (DFT) calculations revealed that Ru doping significantly enhanced the proton transfer ability while simultaneously weakens the adsorption capacity of monoethanolamine (MEA) on the catalyst surface. Moreover, the stronger photothermal effect introduced by Ru leads to an increase in the surface temperature of the catalyst, which is key to the faster and efficient desorption of CO 2 . This work provides a new approach to improve the proton transfer ability of catalysts and offers a novel photothermal coupled catalytic scheme for CO 2 desorption in organic amine carbon capture technology.
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Inorganic Chemistry Frontiers
·
2024
·
IF 6.1
Lu Yan,Yue Shen,Zidan Zou,Xiao Zhang,Zhixin Yu,Guozhong Wang,Chun Chen
Hydrogenation of aromatic rings can be used not only for synthesis fine chemicals, but also for hydrogen storage and transportation using organic hydride. In this paper, yolk-shell structural SiO2@Ru@NC catalyst, which was successfully synthesized by a strategy of combining modified Stöber and vacuum-assisted impregnation, revealed excellent catalytic activity in dimethyl terephthalate (DMT) hydrogenation to dimethyl 1,4-cyclohexanedicarboxylate (DMCD), which is a green chemical reagent and precursor for high-value chemicals. Characterization results showed that highly dispersed Ru NPs with subnanometer size distribution were encapsulated in yolk-shell nanoarchitecture and the mesoporous shell could ensure unhindered diffusion of reactant molecules. Moreover, yolk-shell structure-induced interaction of Ru and carbon shell allowed for tuning electronic structure of Ru species, which in turn could regulate catalytic properties. The yolk-shell nanoarchitecture catalyst offers advantages of low active metal loading, excellent activity and stability, thus can expand application of ultra-low loaded precious metal catalysts in catalytic conversion of aromatic compounds.
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