INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Jiayao Chen,Yuan Gao,Wenwen Yang,Zhiwei Li,Kun Xiong
Designing highly active and durable catalysts is considered to be crucial for enhancing hydrogen evolution reaction (HER) from water electrolysis . Although some studies indicate that anatase TiO 2 is a promising candidate for electrolytic hydrogen evolution reaction, the influence of different crystalline phases of TiO 2 on the supported Ru catalysts for electrocatalytic HER performance is rarely systematically explored. Herein, a series of Ru/TiO 2 -X (X = R (Rutile), A (Anatase), and P25) catalysts were prepared to investigate the influence of the rutile and anatase phases of TiO 2 on the catalytic activity of Ru catalysts in HER. The findings demonstrate that the HER activity is much affected by the variation of the titania structure, when other factors are kept constant. The 15Ru/TiO 2 -R-H 2 has superior HER performance with a small overpotential of 63 mV to achieve a current density of 10 mA cm −2 in acidic electrolyte and 99 mV in alkaline electrolyte compared to 15Ru/TiO 2 -A-H 2 and 15Ru/TiO 2 -P25-H 2 . This might be attributed to the faster electron transfer and lower Fermi level caused by the oxygen vacancy (V O ) and strong metal-support interaction (SMSI), along with the exposure of active sites afforded by the highly dispersed ruthenium nanoparticles on the rutile TiO 2 . Our results indicate that the presence of rutile TiO 2 support alone is adequate to maintain Ru in its most active form and make it a more performing catalyst, compared to anatase titania and P25.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wentao Wang,Qizhu Qian,Yapeng Li,Yin Zhu,Yafei Feng,Mingyu Cheng,Huaikun Zhang,Yangyang Zhang,Genqiang Zhang
Hydrazine oxidation-assisted water electrolysis provides a promising way for the energy-efficient electrochemical hydrogen (H2) and synchronous decomposition of hydrazine-rich wastewater, but the development of highly active catalysts still remains a great challenge. Here, we demonstrate the robust and highly active Ru nanoparticles supported on the hollow N-doped carbon microtube (denoted as Ru NPs/H-NCMT) composite structure as HER and HzOR bifunctional electrocatalysts. Thanks to such unique hierarchical architectures, the as-synthesized Ru NPs/H-NCMTs exhibit prominent electrocatalytic activity in the alkaline condition, which needs a low overpotential of 29 mV at 10 mA cm–2 for HER and an ultrasmall working potential of −0.06 V (vs RHE) to attain the same current density for HzOR. In addition, assembling a two-electrode hybrid electrolyzer using as-prepared Ru NPs/H-NCMT catalysts shows a small cell voltage of mere 0.108 V at 100 mA cm–2, as well as the remarkable long-term stability. Density functional theory calculations further reveal that the Ru NPs serve as the active sites for both the HER and HzOR in the nanocomposite, which facilitates the adsorption of H atoms and hydrazine dehydrogenation kinetics, thus enhancing the performances of HER and HzOR. This work paves a novel avenue to develop efficient and stable electrocatalysts toward HER and HzOR that promises energy-saving hybrid water electrolysis electrochemical H2 production.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Ying Yu,Xiaodan Wang,Mingyang Li,Dengyong Liu
5′-Guanosine monophosphate (5′-GMP) is one main source of freshness in broths. Herein, an electrochemical platform based on a novel ternary nanocomposite glassy carbon electrode modified with advantageously-united gold nanoparticles, 2,2′-bipyridine hydrated ruthenium (Ru(bpy) 2 Cl 2 ) and sulfonated multi-walled carbon nanotubes (SMWCNTs)was prepared and used to detect 5′-GMP. After conditions optimization, the best performance of the electrochemical sensor was found in acidic media, including high specificity, sensitivity and selectivity. The electrochemical sensor exhibited a wide linear range under the optimal conditions. The enhanced sensitivity of this sensor was attributed to the Ru(bpy) 2 Cl 2 and functionalized SMWCNTs that provided high electrical conductivity and electrocatalytic properties during electrochemical reaction . Precise analysis of 5′-GMP in actual broth samples showed satisfactory recovery. Thus, the sensor can be used in the market and food enterprises.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Zhang,Rui Li,Luyao Cui,Zijun Sun,Lijun Guo,Xiaochao Zhang,Yunfang Wang,Yawen Wang,Zhuobin Yu,Tao Lei,Xuan Jian,Xiaoming Gao,Caimei Fan,Jianxin Liu
Synergistic water activation and nitrogen reduction process is significant to the photocatalytic ammonia synthesis reaction, in which the obtainment of active hydrogen (H*) from H 2 O dissociation and then transfer to N 2 activation site is essential. Herein, the oxygen vacancies (OVs) enhanced hydrogen spillover is used to increase the H* transfer between the H 2 O activation site (Ru) and the N 2 activation site (OVs-rich W 18 O 49 ). Results shown that the OVs-rich Ru/W 18 O 49 achieves high activity for NH 3 production with a yield of 222.75 µmol‧g −1 ‧h −1 , which is 5.60 folds of the OVs-deficient Ru/W 18 O 49 . Control experiments, characterization, and theoretical calculation made it clear that OVs played crucial roles in enhancing the hydrogen spillover by modifying the support's Gibbs free energy for hydrogen adsorption and lowering the barrier of H* migration. Finally, the detail mechanism was explained from a new perspective. This strategy may provide new insights for other hydrogenation reactions under mild conditions.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2018
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IF 2.891
Sujitraj Sheth,Mengyuan Li,Qijun Song
Due to clinical importance, detection of dopamine by using easy and rapid method is still ongoing challenge. Here we present a simple and quite efficient method for dopamine (DA) detection in alkalescent medium using in situ prepared Ru(II) complex and sodium dodecyl benzyl sulfonate (SDBS) as highly luminescent luminophore. The luminescence enhancement in the Ru(II) complex (Ru-CIP) has been observed in the miceller medium formed by SDBS. The capability to successively quench the luminescence intensity has been tested for variety of molecules and only dopamine as analyte found to be able to quench luminescence effectively. Hence selective quenching of luminescence by dopamine was used as a tool to detect dopamine and two linear concentration ranges has been established from 0.1 μM to 1μM and from 2 μM to 10 μM with limit of detection (LOD) is 6.6 nM (S/N = 3). Spectral evidence showed that luminescence quenching mechanism arose via Forster resonance energy transfer (FRET) among oxidized DA (i.e. DA quinone) and in situ generated Ru-CIP and SDBS assembly. Due to ultra sensitivity and high selectivity of the prescribed (Ru-CIP-SDBS) luminescent probe has a strong potential for practical analytical application in clinical diagnosis.
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Asian Journal of Organic Chemistry
·
2018
·Vol. 7
·期 10
·2039-2044
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IF 2.496
Qian-Qian Huang,Wei-Qiang Yu,Xiao-Lin Luo,Jin Gao,Jie Xu
Graphical An alternative method for glycerol hydrogenolysis to CH 4 and ethylene glycol that proceeds through preferential C−C bonds cleavage catalyzed by highly-dispersed Ru catalysts with tunable particle sizes via carbothermal reduction has been reported. An alternative method for the conversion of crude glycerol was proposed to produce renewable energy methane and high-value chemical ethylene glycol through preferential cleavage of C−C bonds, catalyzed by highly dispersed Ru-based catalysts prepared by carbothermal reduction. It was found that the Ru particles size could be tuned by adjusting the reduction temperature, and the size firstly decreased then increased with raising of the temperature of carbothermal reduction. This resulted in the opposite tendency of catalytic performance against the Ru particle sizes in hydrogenolysis of glycerol, in which the glycerol conversion and yield of C−C bond cleavage increased firstly and then decreased. Ru catalysts carbothermal reduced at 450 °C possessed highly dispersed Ru nanoparticles with uniform particle sizes about 1.0 nm that showed high hydrogenation activity and selectivity of C−C bond cleavage as well as good stability that could be recycled in aqueous phase hydrogenolysis of glycerol.
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NANOTECHNOLOGY
·
2018
·Vol. 29
·期 7
·075708
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IF 3.404
Hengcong Tao,Jingjing Ding,Chao Xie,Yunnan Gao,Jinliang Song,Zhenyu Sun
We demonstrate a facile and versatile method to grow Ru particles uniformly on pristine few-layer graphene (FLG) in supercritical diethylamine. In particular, a large number of Ru subnanometer clusters less than 1.0 nm were observed. The particle size can be tuned by manipulating the loading content of Ru and controlling the reaction temperature. The resulting Ru/FLG showed remarkably high activity, selectivity, and reusability towards the hydrogenation of levulinic acid to γ-valerolactone. This method is flexible, and can be extended to the synthesis of a variety of other ultrafine metal particles supported on FLG.
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BIOSENSORS & BIOELECTRONICS
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2017
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IF 7.78
Haiyan Wang,Chunling Qi,Wenhuan He,Minghui Wang,Wenjing Jiang,Huanshun Yin,Shiyun Ai
A novel, simple and sensitive photoelectrochemical (PEC) immunosensing platform was constructed for detecting N 6 -methyladenosine (m 6 A) based on the carboxylated CN and avidin functionalized [email protected] 2 (ARS) nanocomposite . Herein, the N 6 -methyladenosine-5′-triphosphate (m 6 ATP) was selected as the detection target molecule, m 6 A antibody was used as recognition unit for m 6 A, the carboxylated g-C 3 N 4 (CN) was not only used as the photoactive substance, but the substrate for the m 6 A antibody immobilization , ARS was synthesized and used as signal amplification unit to improve the photocurrent of CN, Phos-tag-biotin was employed as bridge of m 6 ATP and [email protected] 2 through the specific interaction between phosphate group of m 6 ATP and Phos-tag, biotin and avidin, respectively. Under the optimal condition, the fabricated PEC biosensor showed a linear range of 0.01–10 nM and high detection sensitivity with low detection limit of 3.23 pM for m 6 ATP. Besides, the developed strategy was also successfully applied to evaluate the content of m 6 A in human serum samples.
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SENSORS AND ACTUATORS B-CHEMICAL
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2013
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IF 3.535
Meng Li,Hongmei Yang,Chao Ma,Yan Zhang,Shenguang Ge,Jinghua Yu,Mei Yan
In this paper, a novel and sensitive signal-off electrochemiluminescence (ECL) aptasensor was proposed for the detection of adenosine triphosphate (ATP) on a nanoporous gold (NPG) modified glassy carbon electrode. The NPG was easily synthesized by a selective dissolution of silver from silver/gold alloy in nitric acid . The ECL aptasensor consisted of two main elements: an ECL substrate, made by modifying the amino group functionalized Ru(bpy) 3 2+ -doped silica (Ru-silica), and an ECL intensity switch, which contains two probes, split from one aptamer. The first probe (ssDNA1) was functionalized with a thiol group at one end and attached to Ru-silica through the linking agent of N-succinimidyl-4-(N-maleimidomethyl)cyclohexane-1-carboxylate. The other one (ssDNA2) is ferrocene-labeled probe, which was functionalized with ferrocene tag at the amino group functionalized end. We demonstrated that the ssDNA1/ATP/ssDNA2 sandwich composites layer could be formed in the presence of ATP, and lead to a quenching of Ru(bpy) 3 2+ . However, only a slight decrease could be observed in the absence of ATP. Under optimal conditions, the proposed biosensor provided a wide linear response range over 0.1 pmol L −1 –10.0 nmol L −1 with a detection limit of 0.03 pmol L −1 .
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Hong Yuan,Bo Chen,Jia-Meng He,Yi-Qing Xie,Xiao-Ran Wang,Yu Wang,Wen-Xin Zhu,Hong-Bing Zang,Zhi-Jun Diao
The high quality liquid products obtained from upgrading of bio-oil through hydrogenation can serve as viable alternatives to fossil fuels, thereby alleviating the strain on energy supply. In this study, a series of titanium-aluminum composite oxides (Ti x Al y O) was prepared by a sol-gel method and used as supports to fabricate ruthenium (Ru)-based catalysts for the hydrogenolysis upgrading of bio-oil. Various techniques, including in situ pyridine adsorption-Fourier-transform infrared spectroscopy (in situ Py-FTIR), in situ CO diffuse-reflectance Fourier-transform infrared spectroscopy (in situ CO DRIFTS), and CO 2 temperature-programmed desorption (CO 2 -TPD), were employed to characterize the physicochemical and electronic structures of the catalysts. Using guaiacol as a model compound for bio-oil, the compositions and structures of the Ti x Al y O supports, as well as the effect of calcination treatment of the supports in an N 2 atmosphere, on the hydrogenolysis reactivity, were investigated in detail. The results indicated that the hydrogenolysis rate of C aromatic −O bonds showed a significant linear correlation with the oxygen vacancy/Lewis acid content. Furthermore, the presence of oxygen vacancies facilitated the formation of small Ru nanoparticles. Importantly, calcination of the support in an N 2 atmosphere facilitated the formation of metal/oxide interface sites in the Ru/Ti 5 Al 5 O-N catalyst, further augmenting its Lewis acidity and reducing the activation energy for the hydrogenolysis of the C aromatic −O bonds. The hydrogenolysis rate of the C aromatic −O bond in guaiacol over the oxygen vacancy-rich catalyst Ru/Ti 5 Al 5 O-N was increased by a factor of 2–4 compared to those over Ru-based catalysts with a single oxide support. This study exemplified a novel strategy of oxygen vacancy-promoted hydrogenolysis upgrading of bio-oil.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Shumin Xie,Mang Niu,Xingyun Li,Yang Lei,Huanfang Zhang,Shuai Xu,Deyu Wang,Sameh M. Osman,Zhi Peng,Yusuke Yamauchi
The development of high-performance electrocatalysts that rival Pt catalysts is crucial for efficiently driving the hydrogen evolution reaction (HER) to produce H2. Herein, we engineer sophisticated interfacial modulation of the Ru catalysts by constructing B, N co-doped porous carbon confined ultra-small MoC quantum dots (MoC@BNC) as an advanced catalyst carrier and stimulator. Combined experimental and theoretical calculations prove enhanced electron interaction between the Ru catalysts and the MoC quantum dots. Additionally, the B, N co-doped carbon substrate further refines the electronic structure of MoC, reinforcing the modulation of Ru catalysts. The Ru/MoC@BNC catalyst embodies a boosted H2O dissociation ability with a lowered H bonding strength, which promises an outstanding HER performance with an overpotential of 14 mV at 10 mA cm−2 in an alkaline solvent. Furthermore, robust catalytic stability is achieved with almost zero deterioration after the cycling test. This result exemplifies the importance of interfacial manipulation of the Ru catalysts to promote HER catalytic performance.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jin-Jian Pan,Jia Huang,Yuan-Hang Qin,Zhen Chen,Li Yang,Cun-Wen Wang,Xingmao Jiang
Ba-based perovskite oxides rich in oxygen vacancies (OVs) are anticipated to possess robust electron-donating capabilities and other favourable properties, rendering them a promising support for Ru catalysts in NH 3 synthesis. Herein, a glucose-urea deep eutectic solvent calcinating method was developed to synthesize an OV-rich BaTiO 3 (BTO-H) support for Ru catalysts. The BTO-H-supported Ru (Ru/BTO-H) catalyst achieves an impressive NH 3 synthesis rate of 5133 μmol g cat –1 h −1 (256.7 mmol g R u –1 h −1 ) at 400 °C and 0.1 MPa, surpassing the performance of Ru catalysts supported on OV-poor BTO supports and other supported Ru catalysts. Physical characterizations and kinetic experiments reveal the multifaceted influence of OVs on enhancing the catalytic performance of Ru/BTO-H in NH 3 synthesis. OVs serve as electron donors to Ru catalyst, facilitating the activation and dissociation of N 2 . Simultaneously, OVs act as hydrogen acceptors from the Ru surface, mitigating hydrogen poisoning effects. Additionally, OVs stimulate the formation of surface hydrides, not only providing active sites for N 2 activation but also bestowing an electron-donating effect on the supported Ru catalyst. The combined positive effects of OVs establish BTO-H as an outstanding support for Ru catalysts in NH 3 synthesis.
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