Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 7
·3524-3534
·
IF 11.9
Xiaofang Ma,He Xiao,Yang Gao,Man Zhao,Li Zhang,Junming Zhang,Jianfeng Jia,Haishun Wu
Design of efficient and stable hydrogen evolution reaction (HER) electrocatalysts for mass production of hydrogen via electrochemical water splitting is a challenging but urgent task. In this work, a highly dispersed Ru NP catalyst (Ru/HMCs-500) is built using a porous carbon sphere orifice embedded Ru nanoparticle (NP) method and shown to have extremely good HER stability and activity throughout the whole pH range. An ammonia concentration is applied to control the pore size of hollow mesoporous carbon spheres (HMCs) to confine Ru NPs. Noticeably, the mass activities of obtained Ru/HMCs-500 at −50 mV are 1.3 times, 7.0 times, and 3.8 times higher than that of Pt/C in acidic, basic, and neutral solutions, respectively. The characterization results reveal that Ru NPs with an embedded structure are restricted by pores. The high dispersion and anchoring effect ensure the long-term catalytic stability and activity of the catalyst. Metal–support strong interaction (SMSI) optimizes the electronic structure of Ru NPs, which greatly improves their intrinsic activity and reduces the activation energy of the HER. This work enlightens us on how to accurately construct the embedded structure of metal-based materials for enhancing the electrocatalytic HER performance in pH-universal solution.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 47
·期 4
·1685-1690
·
IF 3.925
Jiancheng Lin,Jingjing Liu,Jin Xu
Herein, a versatile electrochemical immunoassay was designed based on an atomically Ru-dispersed nitrogen-doped carbon (Ru–CN) modified disposable screen-printed carbon electrode (SPCE) for sensitive and specific screening of low-abundance influenza A (H1N1) virus with an innovative split-type strategy. Atomic-level Ru–CN can be obtained after pyrolysis of an acetylacetone ruthenium-encapsulated metal–organic framework (zeolite imidazolate framework 8, ZIF-8), which shows a good electrochemical response to ascorbic acid. To achieve H1N1 detection, an alkaline phosphatase (ALP)-loaded sandwich immunoassay was used to generate ascorbic acid in a 96-well plate, which is then dropped onto the Ru–CN modified disposable SPCE to generate a significant current signal using differential pulse voltammetry (DPV). Under optimal conditions, the DPV peak currents were positively correlated with the H1N1 influenza virus concentration in the dynamic working range of 1.0 ng mL−1 to 10 000 ng mL−1 with a limit of detection (LOD) of 0.28 ng mL−1. During the detection of the H1N1 influenza virus, we also focused on the analysis performance of the sensor system and found that the platform has good reproducibility, high specificity, and acceptable stability. Impressively, the proposed sensing system is equivalent to the commercial detection method (ELISA) in the measurement of the H1N1 influenza virus from clinical samples, which further confirms the accuracy of the Ru–CN-based electrochemical immunoassay method. This enhanced analytical performance through atomic-level dispersed metals gives a new horizon to develop highly sensitive electrochemical immunoassays in the field of early detection of epidemic viruses.
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2023
·Vol. 25
·期 21
·8531-8538
·
IF 9.8
Rong Fu,Yan Wang,Guangming Wang,Qingyun Zhan,Lili Zhang,Le Liu
Well-crafted semiconductors exhibiting favorable band structures and strong electron-donating properties can provide a viable pathway for solar-driven nitrogen activation under ambient conditions. In this study, we demonstrate that the nitrogen photo-fixation process can be enhanced by introducing oxygen vacancies and a Ru co-catalyst. The Ru-loaded ZrO2−x photocatalyst achieved an impressive NH3 production rate of 3256 μg g−1 h−1 under visible light irradiation (at 400 nm). Defective ZrO2−x with its enhanced reducing ability and narrow band gap possesses a low work function and excellent electron-donating capability, resulting in remarkable photocatalytic performance for ammonia synthesis under visible light. The supported Ru co-catalyst induces upward band bending in defective ZrO2−x, forming an interfacial Schottky barrier that facilitates the separation of photogenerated charge carriers and provides energetic electrons for nitrogen activation. Mott–Schottky photocatalysts with enhanced back donation ability establish a one-way channel for the transmission of photoexcited electrons, thereby further improving the photocatalytic performance of ammonia synthesis at room temperature.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Ying Yang,Dongcheng Ren,ChunLi Shang,Zhongzhen Ding,Xinruo Luo
Direct conversion of cellulose to high yield 1,2-propylene glycol (1,2-PG) is amazing in the biomass valorization to diols, since this process is atom-economic, carbon neutral, and the produced 1,2-PG has a large market demand. However, it is very challenging to control cellulose hydrogenolysis owing to high reactivity of intermediates (like glucose) and metal-acid repelling, leading to decreased selectivity of metal-acid multi-functional catalysts. Aimed at this, we herein developed a highly selective metal-acid catalyst (Ru/NC@void@MC-SO 3 H) with site isolated Ru clusters (1.4 nm) on the core and sulfoacids on the shell in a yolk-shell nanoreactor by a layer-by-layer assembly before chemical transformation. The spatial isolation of metal and acid sites integrated in a mesoporous yolk-shell nanoreactor not only facilitates the metal-acid synergism in hydrolysis, isomerization/hydrogenolysis and hydrogenation cascade reactions, but also provides a designated diffusion pathway that is favorable for reaction species. As expected, the elaborately fabricated Ru/NC@void@MC-SO 3 H proves to be highly selective to 1,2- PG (38 % yield), delivering a productivity of 342.86 mol h −1 g Ru –1 and an extremely high turnover number of 173264, outperforming the state-of-art metal-acid catalysts for cellulose hydrogenolysis to 1,2-PG. Our characterization and performance test suggest that sulfoacids are mainly responsible for cellulose hydrolysis, while N -stabilized Ru centers contribute to the glucose isomerization to fructose and its further hydrogenolysis to dihydroxyacetone, followed by hydrogenation to 1,2-PG on metallic Ru species. The acidity and basicity optimized for site isolated Ru/NC@void@MC-SO 3 H is beneficial to balance intermediate reactions, rendering a higher selectivity to target 1,2-PG. The concept illustrated in this study will provide a guide for the development of other site isolated multi- functional catalysts towards cellulosic biomass conversion and other cascade reactions.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Nano
·
2022
·
IF 13.364
H. Wang,Y. Liu,H. Wang,J. Song,D. Ma,Z. Dai
Efficient utilization of hydrocarbon fuels holds great significance for the current vehicle low-emission requirements and future carbon-neutral society. However, the scenario that limits the effective fuel use and combustion is the present undesirable hydrocarbon-cracking catalysts of low activity, serious coking, and easy degradation. To tackle these issues, we rationally designed and synthesized an active, anti-coking, and recyclable all-in-one zeolite@Ru–Al 2 O 3 catalyst on FeCrAl support by steam-assisted crystallization and atomic layer deposition . Ru nanoclusters dispersedly on ZSM-5 can boost the catalytic efficiency for hydrocarbon cracking and anti-coking, while the protective Al 2 O 3 thin layers further ensure the reusable economy. As for n-dodecane (C 12 H 26 ) cracking reaction, the ZSM-5@Ru–Al 2 O 3 showed a high unit activity up to 0.1253%·ml·mg −1 ·min −1 , low-carbon deposition rate, and the enhanced first-cycle carbon removal rate of 78.3% for recyclable use. Density functional theory (DFT) calculations have further confirmed that high catalytic efficiency and low-carbon deposition benefit from the timely adsorption of C 12 H 26 and timely transfer of reactant products at the composite interface. This work opens interesting possibilities for the rational design and fabrication of high-efficient, anti-coking, and recyclable hydrocarbon cracking catalysts through multifunctional structural regulations.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2022
·
IF 4.177
Kang Hu,Ping Liu,Ziqing Zhang,Ji Bian,Guowei Wang,Hongjun Wu,Hui Xu,Liqiang Jing
g-C3N4 is a promising photocatalyst for CO2 conversion owing to its outstanding reduction potential. However, its shallow valence band position and sluggish water oxidation reaction restrict the overall CO2 photoreduction process. Herein, g-C3N4 nanosheets are first doped with B through thermal treatment of mixed NaBH4 and subsequently modified with highly dispersed Ru-oxo clusters by using tailored chitosan oligomers. The optimal Ru-oxo modified B-doped g-C3N4 exhibits an exceptional photocatalytic CO2 conversion rate with 22-fold improvement compared with pristine CN. Based on the results of electron paramagnetic resonance, atmosphere-controlled surface photovoltage spectroscopy, in situ diffuse reflectance infrared Fourier transform spectroscopy, etc., it is confirmed that the improved photoactivities are attributed to the downward shift of the valence band to obtain the strong driving force for water oxidation along with extension of the visible light response region by B doping and to the capture of photogenerated holes to enhance charge separation and then to accelerate the water oxidation process from the modified Ru-oxo clusters.
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Qiao-Fen Pan,Hai-Feng Jiao,Hua Liu,Jin-Jie You,Ai-Li Sun,Ze-Ming Zhang,Xi-Zhi Shi
A novel molecularly imprinted electrochemiluminescence (MIECL) sensor based on the luminescence of molecularly imprinted polymer-perovskite (MIP-CsPbBr 3 ) layer and Ru(bpy) 3 2+ was fabricated for simazine detection. MIP-CsPbBr 3 layers were immobilized onto the surface of glassy carbon electrode as the capture and signal amplification probe, and Ru(bpy) 3 2+ and co-reactant tripropylamine exhibited stronger electrochemiluminescence (ECL) emission. Under optimal conditions, the ECL signal of the MIECL sensor was linearly quenched, with the logarithm of simazine concentration ranging from 0.1 μg/L to 500.0 μg/L, correlation coefficient of 0.9947, and limit of detection of 0.06 μg/L. The practicality of the developed MIECL sensor method for simazine determination in aquatic samples was validated. Excellent recoveries of 86.5 %–103.9 % with relative standard deviation below 1.6 % were obtained for fish and shrimp samples at three different spiked concentrations. The MIECL sensor exhibited excellent selectivity , sensitivity, reproducibility, accuracy, and precision for simazine determination in actual aquatic samples.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Min Jiang,Rui Dong,Hanxiao Liao,Yong Liu,Yuan Wang,Pengfei Tan,Jun Pan
Rational fabrication of an electrocatalyst with excellent stability, conductivity, and activity is urgently demanded for oxygen evolution reaction (OER). In this work, Ru-regulated hierarchical CoFe/CoFe 2 O 4 nanoparticles with graphitic carbon shells were successfully fabricated via self-assembling and vapor reduction strategies. Our investigation uncovers high concentrations of octahedral Co 3+ sites in electrocatalysts can be triumphantly acquired via moderate Ru doping, which could give rise to excellent electrocatalytic activities during OER. In addition, the design of CoFe alloys and graphitic carbon shells can compensate for the weak conductivity of cobalt ferrites. Based on the intrinsic stability, improved conductivity and activity, the as-prepared electrocatalyst yields a low overpotential of 237 mV at 10 mA cm −2 and a small Tafel slope of 47 mV dec −1 in 1.0 M KOH electrolyte, exhibiting outstanding electrocatalytic activities for OER.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Qijun Tang,Peiyao Xiong,Haiqiang Wang,Zhongbiao Wu
Photocatalytic CO 2 reduction to produce value-added products is considered a promising solution to solve the global energy crisis and the greenhouse effect. In this study, Ti 3 CN MXene was synthesized using a Lewis acidic etching method without the usage of toxic hydrofluoric acid (HF). Ti 3 CN MXene was then used as a support for the in situ hydrothermal growth of TiO 2 and Ru nanoparticles. In the presence of 0.5 wt% Ru, Ru-Ti 3 CN-TiO 2 shows CO and CH 4 production rates of 99.58 and 8.97 μmol/g, respectively, in 5 h under Xenon lamp irradiation, more than 20.5 and 9.3 times that of commercial P25. The enhancement in photocatalytic activity was attributed to the synergy between the in-situ growth of TiO 2 on Ti 3 CN MXene and Ru nanoparticles. It was proven experimentally that Ti 3 CN MXene can provide abundant pathways for electron transfer. The separation and transfer of the photo-induced charge were further increased with the help of Ru and Ti 3 CN MXene, leaving more electrons to participate in the subsequent CO 2 reduction reaction. We believe that this work will encourage more attention to designing environment-friendly MXene-based photocatalysts for CO 2 photoreduction using the non-HF method.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
·
2022
·
IF 12.781
Ran Xi,Yiwei Tang,Richard Lee Smith,Xiaoning Liu,Le Liu,Xinhua Qi
Ni–Ru bimetallic porous carbon sphere (Ni–Ru@PCS) catalysts were synthesized via formaldehyde-assisted, metal-coordinated crosslinking sol–gel chemistry, in which biomass-derived tannic acid and F127 surfactant were used as carbon precursor and soft template, respectively, and Ni 2+ and Ru 3+ were used as cross-linkers. In the developed method, Ni–Ru particles became uniformly dispersed in the carbon skeleton due to strong coordination bonds between metal ions (Ni 2+ and Ru 3+ ) and tannic acid molecules and bimetal interactions. The as-synthesized Ni–Ru 10:1 @PCS catalyst with a loading Ni:Ru mole ratio of 10:1 was applied for the selective hydrogenation of glucose to sorbitol, and provided 99% glucose conversion with a sorbitol selectivity of 100% at 140 °C in 150 min reaction time and exhibited good stability and recyclability in which sorbitol yield remained at 98% after 4 cycles with little or no metal agglomeration. The catalyst was applied to glucose solutions as high as 20 wt% with 97% sorbitol yields being obtained at 140 °C in 20 h. The developed bimetallic porous carbon sphere catalysts take advantage of sustainably-derived materials in their structure and are applicable to related biomass conversion reactions.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 11
·15337-15346
·
IF 5.19
Yang Zhen-xing,Shang Jie,Yan Guang-xu,Wang Yu-xian,Guo Shao-hui
In this paper, Pd-Sn modified Ru-Ir electrode was prepared by thermal oxidation method, and the effects of doping amount of Pd-Sn and synthesis conditions on Pd-Sn modified Ru-Ir electrode performance were studied. Linear sweep voltammetry(LSV), cyclic voltammetry(CV), and the Tafel curve were used to study the electrochemical performance of the Pd-Sn modified Ru-Ir electrode materials. The effects of the doping amount of Pd-Sn on the microstructure and valence states of Pd-Sn modified Ru-Ir electrode materials were investigated by SEM, TEM, XRD, and XPS. When the mass of Pd-Sn accounted for 1.5% of the total mass of the elements, the molar ratio of Ru-Ir was 2:1, and the molar ratio of Pd-Sn was 3:1; the LSV, CV, and the Tafel curves indicated that Pd-Sn modified Ru-Ir electrode had the lowest chlorine evolution potential (1.0640 V vs. SCE), the best CV curve coincidence, and the smallest corrosion current density (6.5 × 10 −4 A/cm 2 ), showing the best chlorine evolution performance, the best durability, and corrosion resistance; the characterization of SEM, TEM, XRD, and XPS showed that Pd-Sn was successfully doped into Ru-Ir electrode materials; the crystallinity of Pd-Sn modified Ru-Ir electrode was the highest, and the binding energy was the lowest, but the crystal form of Ru-Ir solid solution did not have changed. The optimal synthesis conditions of Pd-Sn modified Ru-Ir electrode material were as follows: Pd-Sn molar ratio was 3:1, calcination temperature was 500 ℃, calcination time was 4 h, and water was used as solvent. Pd-Sn modified Ru-Ir electrode can efficiently treat high chlorine ammonia–nitrogen wastewater, when the reaction volume was 200 mL, the initial concentration of NH 3 -N was 100 mg/L, the concentration of chloride ion was 5000 mg/L, the current was 0.75 A, and the reaction time was 40 min; the removal rate of ammonia nitrogen can reach 100%. Responsible editor: Weiming Zhang.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xuzhuo Sun,Wenhui Li,Jing Chen,Xinli Yang,Baofan Wu,Zhengxi Wang,Bo Li,Haibo Zhang
As a promising dopant , electron deficient B atom not only tunes the electronic structure of electrocatalysts for improving their intrinsic catalytic activities, but also combines with hydroxy radical as strong adsorption sites for accelerating the water dissociation during the hydrogen evolution reaction (HER). In this paper, we report an electrocatalyst based on boron-modified Ru anchored on carbon nanotubes (B-Ru@CNT) that shows impressive HER activity in acidic and alkaline media. The boron-rich closo -[B 12 H 12 ] 2- borane was selected as a moderately strong reductant for the in situ reduction of a Ru salt, which yielded B-doped Ru nanoparticles . The experimental and theoretical results indicate that the incorporation of B not only weakens the Ru-H bond and downshifts the d-bond centre of Ru from the Fermi level by reducing the electron density at Ru but also accelerates the water dissociation reaction by providing B sites, which strongly adsorb OH* intermediates, and nearby Ru sites, which act as sites for the adsorption of the H* intermediate, thus boosting the HER performance and enhancing the HER kinetics. As a result of the tuning of the electronic structure via B doping, B-Ru@CNT showed excellent HER performance, yielding overpotentials of 17 and 62 mV at a current density of 10 mA cm −2 in alkaline and acidic solutions, respectively. These results indicate that our synthetic method is a promising route to B-doped metallic Ru with enhanced pH-independent HER performance.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）