GREEN CHEMISTRY
·
2016
·Vol. 18
·期 11
·3370-3377
·
IF 8.506
Wenjing Yang,Haiyang Cheng,Bin Zhang,Yan Li,Tong Liu,Mingli Lan,Yancun Yu,Chao Zhang,Weiwei Lin,Shin-ichiro Fujita,Masahiko Arai,Fengyu Zhao
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was studied with a homogeneous RuCl2(PPh3)3 catalyst in supercritical CO2 (scCO2). The conversion of LA was observed to increase with CO2 pressure and the possible reasons for this rate acceleration were discussed, including the molecular interactions of CO2 with the reacting and catalytic species as well as the acidity and phase behavior of the reaction mixture. The interaction between CO2 and RuCl2(PPh3)3 was significant, which resulted in the production of an active RuHCl(CO)(PPh3)3 complex and thus enhanced the rate of hydrogenation in the presence of CO2.
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ANALYTICAL CHEMISTRY
·
2016
·
IF 5.886
Hui Zhang,Huilei Dong,Guoqing Yang,Hongfei Chen,Chenxin Cai
Effective detection of DNA methyltransferase (DNMT) activity is significant for cancer research. Herein, we developed a sensitive electroanalytical method to detect human DNA (cytosine-5)–methyltransferase 1 (DNMT1) from crude lysates of cancer cells. In this assay, capture DNA having a preferred DNMT1 methylation site was immobilized on a gold electrode and then hybridized with gold nanoparticle (Au NP)–DNA complexes. The modified electrodes were equilibrated with the lysate and then incubated with methylation-sensitive restriction enzyme. If the lysate was negative for DNMT1 activity, the Au NP–DNA complexes would be cut by the restriction enzyme and released from the electrode. Conversely, restriction enzyme cleavage would be blocked by the fully methylated duplexes, and the Au NP–DNA complexes would remain on the electrode. Electroactive Ru(NH3)63+ was used as the signal reporter, because of its electrostatic attraction to DNA, resulting in an electrochemical signal. Since the electrochemical signal reflects the amount of Ru(III) redox and the amount of Ru(III) redox is correlated with the activity of DNMT1, the activity of DNMT1 is proportional to the electrochemical signal. The signal could be amplified by the numerous DNAs on the Au NPs and further amplified by Ru(III) redox recycling. With this method, a detection limit down to 0.3 U/mL for pure DNMT1 and 8 MCF-7 cells was achieved. DNMT1 activities of different cell lines were also successfully evaluated.
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PubMed
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ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Shan Gao,Tinghong Lu,Xiaohan Zhu,Fengli Yu,Bing Yuan
A catalytic system of Ru nanoparticles (NPs), Ru@SLSaq, dispersed in water was developed by employing sodium lignosulfonate (SLS) to reduce and stabilize ruthenium(III) cation heptaacetate (Ru3O(OAc)7) in an aqueous solution. This Ru@SLSaq catalytic system enabled the efficient hydrogenation of diphenylmethane (DPM) and o-hydroxydiphenylmethane (o-HDPM), yielding dicyclohexylmethane (DCHM) and perhydrofluorene (PHF), respectively. Characterization using UV–vis, FT-IR, Raman spectroscopy, HR-TEM, CO chemisorption, DLS, XRD, and XPS demonstrated that SLS effectively replaces the axial acetate ligands of Ru3O(OAc)7, reduces Ru in situ through the phenolic hydroxyls in its macromolecular structure, and maintains the stability of its core structure, thereby preventing the aggregation of generated Ru NPs. The obtained Ru NPs, predominantly in the Ru0 state with a Ru (100) lattice plane, were uniformly dispersed in the aqueous phase, exhibiting an average particle size of 2–3 nm. Ru@SLSaq displayed excellent catalytic activity for the hydrogenation of DPM and o-HDPM, achieving yields of 96.6% and 97.0% for DCHM and PHF, respectively, under mild conditions (n(substrate)/n(Ru) = 750, hydrogen pressure of 1.5 MPa, at 80 °C for 4 h). The calculated apparent activation energies (Ea) for the two reactions were found to be 46.5 kJ·mol–1 and 75.3 kJ·mol–1, respectively, and the catalytic system demonstrated good cycling stability. Experimental results, supported by DFT calculations, indicate that the complete hydrogenation processes of DPM and o-HDPM occur on the surface of Ru NPs via monophenyl ring adsorption, exhibiting small energy barrier differences across various pathways.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Wu,Jiangfu Zheng,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan
Design of green and low-cost single-atom catalysts (SACs) with high-performance is key to moving photocatalytic degradation of antibiotics toward applications. In order to achieve SACs for large-scale manufacturing, we prepared ultrathin flake carbon nitride (FCN) by low-energy-consuming physical knockout means, and also applied an in situ growth strategy with stable and easy-operating effect to anchor the Ru element on FCN in the form of single atom. Notably, in the PMS/Vis/0.5Ru-FCN system, the degradation rate of tetracycline achieved 100 % in just five minutes, with an apparent rate constant of 0.236 min −1 . Ru-FCN exhibits selective and stable determination due to narrow bandgap, unique photoresponsivity and low photogenerated carrier complexation rate. Mechanism investigation reveal that Ru-N 4 sites accelerated the electron transfer between Ru-FCN and PMS, while the low oxidation state of Ru elements reduced the risk for metal corrosion. DFT calculations predict the attack sites of reactive oxygen species. This work provides a rational explanation for the charge transfer and resistance to external disturbance by Ru single atom, and it also provides a new direction to enhance the efficiency of water treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Zunpeng Hu,Qian Geng,Senjie Dong,Minghui Wang,Yuqian Song,Wenjing Sun,Han Diao,Ding Yuan
Exploiting the high-entropy alloy (HEA) electrocatalysts with the synergistic effect of multi-metal components is an effective approach to address the slow kinetics and undesirable stability of the oxygen evolution reaction (OER) in Zn-air batteries (ZABs), but still faces many challenges. In this study, a multimetallic Metal-organic framework (MOF)-derived HEA catalyst was successfully fabricated on carbon fiber as a flexible self-supporting electrode (denoted as CC@FeCoNiMoRu-HEA/C) for high-performance liquid/flexible ZABs using a facile and cost-effective strategy. The three-dimensional (3D) highly open network framework and hierarchical porous structure accelerate the mass transport of OH − /O 2 and charge transfer. The electronic structure adjustment, lattice defects and high entropy effects enable the CC@FeCoNiMoRu-HEA/C catalysts to perform high OER catalytic activity and strong durability while reducing the Ru content and lowering the economic cost. In situ Raman spectra and XPS results reveal the generation of metal-OOH intermediates on the HEA surface during the OER process. In a practical demonstration, the liquid ZAB assembled with CC@FeCoNiMoRu-HEA/C + Pt/C as the air electrode offers stable open-circuit voltage, large power density, excellent specific capacity and satisfactory cycle life, outperforming the commercial RuO 2 + Pt/C-based reference ZAB. More attractively, the flexible solid-state ZAB also achieves fast dynamic response, high peak power density, robust cycling stability as well as favorable mechanical flexibility, indicating a promising application prospect in future flexible electronics and wearable devices. This work provides a viable pathway to develop low precious metal-loaded HEAs as advanced OER self-supporting electrocatalysts and realize high-performance flexible energy storage devices.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Yutong Li,Qiuhong Wei,Haoyue Huang,Shujun Qiu,Yongpeng Xia,Yongjin Zou,Fen Xu,Lixian Sun,Hailiang Chu
Catalyst development remains a critical challenge in chemical hydrogen storage. In particular, efficient, cost-effective heterogeneous catalysts are essential for ammonia borane (NH 3 BH 3 , AB) hydrolysis to enable hydrogen generation. In this study, we developed a self-assembly strategy to fabricate a unique catalyst consisting of a Ru-modified CoN/CoP heterogeneous structure on an MXene support of Ti 3 C 2 T x , creating more multiphase interfaces. Through optimizing experimental conditions, a superior Ru–CoN/CoP@Ti 3 C 2 T x catalyst is achieved, which demonstrates a rapid hydrogen generation rate ( HGR = 1.43 × 10 5 mL min −1 ·g Ru −1 ) and a high turnover frequency ( TOF = 589.7 mol H2 ·mol Ru −1 ·min −1 ) at 25 °C, surpassing most previously reported Ru-based catalysts. The catalytic performance improvement of AB hydrolysis can be ascribed to a much lower apparent activation energy ( E a = 26.3 kJ mol −1 ) and the synergistic effect between CoN/CoP substrates and their interactions with Ru particles and Ti 3 C 2 T x carriers. This study highlights the potential of multi-interface cooperation in advancing the design of heterogeneous catalysts for AB hydrolysis.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Chaojie Cheng,Bicen Yao,Siyu Wu,Wankun Gou,Xiaoai Luo,Xiang Chen,Xianrong Zhang,Hongming Sun,Cheng-Peng Li,Baoguang Mao
Efficient alkaline hydrogen evolution reaction (HER) catalysts are critical for anion exchange membrane water electrolysis (AEMWE). However, the intrinsic scaling relationship between water dissociation and OH desorption fundamentally impedes designing catalysts requiring concurrent superior water dissociation and facile OH desorption. Here, we engineer a superhydrophilic Ru/Cr 2 O 3 heterostructured electrocatalyst through in situ confinement of Ru nanoparticles (5–10 nm) within a Cr 2 O 3 matrix. Acting as a Lewis acid, the Cr 2 O 3 component provides alternative sites for water dissociation, accelerating the Volmer step kinetics and downshifting the Ru d -band center via interfacial charge transfer, while simultaneously adsorbing OH − to form a surface-bound Lewis base that repels excess OH − from Ru sites, thereby suppressing hydroxyl over-adsorption. Concurrently, the superhydrophilic surface architecture promotes efficient hydrogen bubble release, thereby reducing mass transport resistance. As a result, the Ru/Cr 2 O 3 heterostructured electrocatalyst exhibits an ultralow overpotential of 36.7 mV at 10 mA cm −2 and a Tafel slope of 33.2 mV dec −1 . Integrated into an AEMWE device, the electrode delivers 500 mA cm −2 for 2000 h in 1.0 M KOH, underscoring its industrial viability (hydrogen production energy consumption per cubic meter (EW): 3.94 kW h m −3 ; electricity-to-hydrogen energy conversion efficiency (η ETH ): 89%@80 °C).
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yong Zhou,Yiyang Zhou,Jiamei Liu,Yanan Zhu,Bin Yang,Jian Lv,Bing Li,Xiaoyang Liu
The production and utilization of hydrogen energy are important for achieving green and sustainable development and are among the most crucial strategies for realizing the efficient use of renewable energy. Electrolysis of water is a promising way to obtain clean hydrogen energy. Ru-loaded carbon materials have a wide application prospect in the field of water electrolysis because of their high catalytic activity, good stability, and relatively low cost. In this study, we realized the in situ anchoring of ultrafine Ru nanoparticles on N-doped hollow mesoporous carbon nanospheres (NHMCS) within 15 min via microwave solvothermal pyrolysis of metal carbonyl compounds. We obtained Ru/NHMCS-15–5 catalysts with excellent alkaline hydrogen evolution properties. Cyclic voltammetry (CV) testing in the range of hydrogen desorption potential and electrochemical in-situ Raman spectroscopy indicated that the high electrocatalytic hydrogen reaction activity of Ru/NHMCS-15–5 may stem from its strong H 2 O adsorption capacity and moderate H adsorption strength. Density function theory (DFT) calculation results indicated that the electronic synergetic effect between Ru clusters and NHMCS enable to regulate the charge distribution of Ru/NHMCS and reduce the Gibbs free energy of formation of intermediate species for water dissociation process, thereby accelerating the electrocatalytic kinetics of HER.
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Energy Materials
·
2025
·Vol. 5
·期 8
·N
·
IF 11.2
Baoyu Wang,Ximing Yan,Ming Zhou,Hu Li
Lignin-based guaiacol and its derivatives can be hydrogenated to synthesize 2-methoxycyclohexanols (2-MCHs), widely used in the pharmaceutical industry, while the efficient catalytic conversion of guaiacols into 2-MCHs is challenging due to the interference of the side reaction of CAr-OCH3 bond cleavage. In this work, highly selective hydrogenation of various guaiacyl lignin-derived phenols to 2-MCHs (yields of 86%-97%) was realized over a single-atom Ru-based catalyst (Ru1/o-CeO2-ov) that preferentially exposes the CeO2(111) plane and has abundant oxygen vacancies. Control experiments and mechanism studies expounded that Ru-O-Ce is the active site for hydrogenation of aromatic ring in guaiacols, and the exposed (111) plane and abundant oxygen vacancies of ceria can reduce the activation energy of aromatic ring hydrogenation, thereby enabling guaiacols to generate the corresponding hydrogenated products with high selectivity. Response surface optimization experiments indicated that temperature and time have relatively more significant effects on the 2-MCH yield. Moreover, the Ru1/o-CeO2-ov catalyst exhibited excellent reusability, and was extensively applicable to the hydrogenative dearomatization of different types of lignin-derived phenols, providing a unique solution for upgrading biomass feedstock into specific structural chemicals.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 9
·1-8
·
IF 5.479
Fang Dandan,Zhang Shupei,Dai Hong,Li Xiuhua,Hong Zhensheng,Lin Yanyu
An ultrasensitive competitive-type electrochemiluminescence immunoassay for the mycotoxin zearalenone is described. The method is based on the use of (a) a mimotope peptide that was selected from a phage displayed peptide library and used to substitute ZEN for designing the competitive assay; (b) NiFe 2 O 4 nanotubes with large specific surface area loaded with the ECL probe Ru(bpy) 3 2+ ; and (c) poly(vinylpyrrolidone) (PVP)-assisted synthesis of TiO 2 mesocrystals that acts as the sensing platform and support for antibody immobilization. Under the optimized conditions and at an ECL working potential of 1.1 V, a linear response is found for ZEN in the 0.1 to 1.0 × 10 −5 ng·mL −1 concentration range with a detection limit as low as 3.3 fg·mL −1 .
An ultrasensitive competitive-type electrochemiluminescence (ECL) immunosensor based on mimotope peptide was constructed for the detection of Zearalenone.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shimin Chen,Junnan Han,Zhihuan Li,Zijie Lin,Min Wang,Hucheng Song,Xiaodong Pi,Dongke Li,Linwei Yu,Jun Xu,Kunji Chen
Lithium-carbon dioxide (Li-CO 2 ) batteries using high ion-conductive inorganic molten salt electrolytes, as a kind of promising carbon–neutral technology, have attracted much attention due to the high safety and high energy density. However, sluggish CO 2 reduction reaction (CO 2 RR) and evolution reaction (CO 2 ER) kinetics at cathodes make these batteries losing most of their capacity and power. Here, by engineering the carbon-free three-dimensional (3D) Cr-N-Ru catalysts on silicon nanopillars (Si NP) cathodes, we report a reversible solar photothermal (SPT) molten salt Li-CO 2 battery where solar energy can be efficiently harvested (over 90 % absorption rate from 300 nm to 2500 nm), concentrated and converted to heat. Theoretical simulations support that the 3D Cr-N-Ru catalysts exhibit lower energy barrier and more effectively catalyze the CO 2 RR and CO 2 ER process compared to individual Ru or CrN catalyst. The SPT Li-CO 2 battery shows a reversible cycle lifespan of 83 cycles with lower charge potential (3.2 V) and higher energy efficiency of 72 %, corresponding to ∼ 0.9 V potential gap, than the one using conventional Ru catalysts assembled on Si NP cathode. This battery technology paves the way for developing the next-generation safe and high-energy–density energy storage batteries with carbon–neutral effect.
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FUEL
·
2025
·
IF 7.5
Yongyuan Deng,Yichao Ye,Tao Yin,Jinyao Mai,Zhipeng Tian,Chao Wang,Ying Chen,Zhi Yang,Junling Tu,Riyang Shu
Hydrodeoxygenation (HDO) technology is an essential method for efficiently converting phenolic compounds from biomass into high-quality liquid fuels. Rationally designed catalysts not only significantly enhance stability and reaction rates, but also improve product selectivity and fuel quality. In this study, we proposed a Zr 3+ -defect-rich core–shell structured catalyst Ru@SiO 2 -ZrO 2 and employed it for the HDO of phenolic compounds and lignin pyrolysis oil. Ru nanoparticles are uniformly dispersed and have small particle sizes, showing outstanding catalytic hydrogenation activity. The porous SiO 2 shell possesses a high specific surface area with a high thermal stability, facilitating reactant transport and maintaining catalyst structural integrity. ZrO 2 serves as an acid modifier to enhance the catalyst acidity and promote the deoxygenation procedure. Besides, ZrO 2 enhances the adsorption of phenolic compounds and improves the cleavage of C-O bonds, due to its abundant oxygen vacancies . These factors make the catalyst achieved complete conversion of guaiacol to cyclohexane at mild reaction temperature of 240°C, which is superior to other similar reported results. Compared to conventional supported Ru/SiO 2 -ZrO 2 catalysts, the unique core–shell structure of Ru@SiO 2 -ZrO 2 obtained a sustained catalytic activity after five consecutive recycles without significant deactivation. Moreover, this core–shell catalyst exhibited good HDO performance for various phenolic compounds and lignin pyrolysis oil. The hydrocarbon content increased significantly from 12.7 % to 96.9 % in the upgrading of lignin pyrolysis oil, demonstrating the catalyst’s great potential for future industrial applications.
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