APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinyu Chen,Chuntao Chen,Majeed Muhammad Amjad,Dongping Sun,Bianjing Sun,Kai Zhang
Ruthenium (Ru)-based electrocatalysts are regarded as promising for applications in hydrogen evolution reactions (HER) due to their suitable metal-hydrogen (M-H) bonding energy. However, the strong affinity for adsorbed hydroxyl groups (OH ad ) leads to the inactivation of Ru active sites, leading to unsatisfactory performance in practical HER applications. Herein, a competitive adsorption strategy for the design of crystalline lattice-confined atomic Ru in Tungsten Carbide Nanoislands is reported. Benefiting from the unique "island–multi-atoms" structural features, Ru/WC x exhibits ultra-high mass activity (6000 mA mg −1 ) and excellent turnover frequency (3.89 H 2 −1 ) at − 100 mV vs. RHE, which is 9.5 and 51.2 times higher than commercial 20% Pt/C, respectively. In-depth mechanistic analysis demonstrates that the strength of Ru-OH ad is regulated by the oxophilicity of W atoms and the stronger W-OH ad bond to alleviate Ru site inactivation, thus enhancing the HER activity. This strategy provides a novel concept for designing advanced catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiafeng Xi,Xiaojuan Liu,Liang Zhang,Zuwang Zhang,Junchen Zhuo,Ting Du,Yajie Zhang,Jinyou Duan,Hongliang Dong,Jianlong Wang
Within the illustrious and renowned MXene family, Niobium carbide (Nb 2 C) has astounded researchers by exhibiting an extraordinary level of photothermal conversion efficiency and photothermal stability, all while maintaining the possibility of biodegradability. However, the absence of band gaps hindered Nb 2 C as an attractive photoresponsive material for sterilization purposes. To overcome this obstacle, we engineered a Schottky heterojunction in Nb 2 C by introducing Ru and Bi 2 S 3 based on the work function theory to generate an internal electric field (IEF) in Ru@Bi 2 S 3 /Nb 2 C, thus enhancing the photocatalytic sterilization performance by improving the charge transfer efficiency. The strategic doping of Ru also improved the carrier separation as an electron trap, apart from enhancing the light absorption efficiency by exploiting the Localized Surface Plasmon Resonance (LSPR). The results of Ultraviolet Photoelectron Spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) divulge the stark difference in work function, which facilitates the directional transfer of carrier and subsequently augments the formation of Schottky heterojunction. This unique structure which is beneficial to the generation of reactive oxygen species (ROS). As a result, the in vitro sterilizing efficiency of the Ru@Bi 2 S 3 /Nb 2 C exceeds 99.87%, and in vivo experiments demonstrated wound healing effects in mouse wound models. These results have confirmed the significant implications of Schottky heterojunction for the use of Nb 2 C in the biomedical sector.
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RSC Advances
·
2023
·Vol. 13
·期 30
·21063-21070
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IF 3.9
Yudan Zhong,Yulong Ma,Yonggang Sun,Liqiong Wang,Yuanyuan Li,Feng Lin,Yingbo Zhu
The lignin oil produced by rapid pyrolysis of lignin is considered a promising liquid fuel source. Hydrodeoxygenation (HDO) is a kind of efficient method to upgrade the lignin oil, and a high-performance catalyst is key to the hydrodeoxygenation of lignin oil. In this study, a high dispersion and small size Ru nanoparticle loaded N-doped carbon catalyst was derived by the direct pyrolysis of a mixture of ruthenium trichloride and melamine, and it could efficiently convert lignin oil. The lignin oil was completely transformed at 240 °C and 1 MPa H2, and 36.58% cyclohexane was obtained. The formation, surface area, and nitrogen species of the catalyst could be controlled by changing the precursor of the nitrogen-doped carbon support. The percentage of pyridine nitrogen possessed with melamine as a nitrogen–carbon precursor (31.35%) was much higher than that with urea (16.47%) and dicyandiamide (8.20%) as nitrogen–carbon precursors. The presence of pyridine nitrogen could not only serve as the coordination site for even dispersity and stability of Ru nanoparticles but also regulated the electron density of Ru nanoparticles (NPs) and increased the active site Ru0 through electron transfer.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jing-yi Jiang,Qingyi Li,Wen-chang Wang,Xiao-hui Chen,Zhi-dong Chen
A novel, rapid, and facile electrochemiluminescence sensor which based on carboxylated acetylene black / Ru(bpy) 3 2+ / nafion modified glass carbon electrode (CAB/Ru(bpy) 3 2+ /NAF/GCE) was developed for detecting isoniazid (INH). The CAB/Ru(bpy) 3 2+ /NAF/GCE expresses an efficient electrochemiluminescence response for INH, because of the brilliant luminous efficiency of Ru(bpy)32+ and admirable electronic transmission of acetylene black. The electrochemiluminescence intensity was quenched significantly with addition of INH. Under the optimal conditions, the sensor for the detection of isoniazid exhibits a wide linear range of 1.0 × 10 -6 ~ 1.0 × 10 -3 mol·L -1 with the detection limit of 5.0 × 10 -7 mol·L -1 . The sensor is expected to be a simple and convenient method for the determination of INH in pharmaceutical samples .
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TALANTA
·
2023
·
IF 6.1
Chen Cui,Xinyao Lin,Jie Lv,Hang Guo,Lu Shen,Guoqiang Xiang,Wenjie Zhao,Dechen Jiang
Designing innovative electrochemiluminescence (ECL) immunosensors is critical for the detection of biomarkers with a low concentration and the precise evaluation of clinical diseases. Herein, a Cu 3 (hexahydroxytriphenylene) 2 (Cu 3 (HHTP) 2 ) nanoflake-based sandwich-type ECL immunosensor was constructed for C-Reactive Protein (CRP) detection. The Cu 3 (HHTP) 2 nanoflake , an electronically conductive metal–organic framework (MOF), has a periodically arranged porous structure with a cavity size of 2 nm, which not only accommodates a large amount of Ru(bpy) 3 2+ but also confines the spatial diffusion of active species. Therefore, the Ru(bpy) 3 2+ -loaded Cu 3 (HHTP) 2 nanocomplex (Ru@CuMOF) as an ECL emitter exhibits an enhanced ECL efficiency. The ECL resonance energy transfer (ECL-RET) was accomplished by combining Ru@CuMOF used as a donor with gold nanoparticles-functionalized graphene oxide nanosheets (GO-Au) utilized as an acceptor. This should be ascribed to the fact that the ECL emission spectrum of Ru@CuMOF shows the strongest signal intensity at 615 nm, overlapping with the absorption spectrum of GO-Au at 580–680 nm. Targeted detection of CRP in human serum samples was achieved by the sandwich-type immunosensor based on the ECL-RET mechanism with a 0.26 pg mL −1 detection limit. The electro-activated hybrids of Cu 3 (HHTP) 2 and ECL emitters provide a new sensing strategy for the high-sensitivity detection of disease markers.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 19
·6336-6346
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IF 6.4
Dong Guo,Chen Chen,Yongqiang Wang,Youke Wang,Conglu Zhang
Two dimensional materials show unique advantages in catalysis. In this work, it was found that melamine could induce the directional growth of cobalt-based catalysts to form an ultra-thin two-dimensional hexagonal nanosheet structure with only 1.5 nm. In addition, these hexagonal nanosheets (HNs) could grow into a microporous structure under high temperature conditions, and the finally formed CoO hexagonal porous nanosheets (HPNs) had a surface area 11.3 times that of the nanoparticles. Embedding 1.25 wt% of monoatomic ruthenium in the CoO HPNs (CoO/Ru1.25% HPNs) allowed the catalyst to have more active charge storage and transfer centers. The results showed that the overpotential of CoO/Ru1.25% HPNs was 64 mV lower than that of CoO nanoparticles at 10 mA cm−2. The Tafel slope of CoO/Ru1.25% HPNs was only half that of CoO nanoparticles, indicating that a small amount of Ru dispersion and the two-dimensional structure control significantly increased the kinetic rate in the oxygen evolution reaction. The DFT results showed that the Ru single atoms in CoO/Ru HPNs (111) possessed the lowest energy barrier (1.19 eV). The Ru single atoms could effectively reconstruct the neighboring localized structure in the formation of ˙OOH, which desirably decreased the free energy of the system.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 36
·8579-8584
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IF 5.16
Min Cheng,Hongbo Geng,Yang Yang,Yufei Zhang,Cheng Chao Li
Graphical Who is the best? Owing to the suitable electronegativity provided by P and synergistic effects of the carbon nanotubes, the RuP 2 /CNT composite achieved high catalytic performance as a hydrogen evolution reaction (HER) electrocatalyst. This may result from the modulation effect of the electronic properties and the depressed adsorption free energy of RuP 2 (see scheme). The utilization of noble-metal catalysts for the hydrogen evolution reaction (HER) provides an efficient strategy for hydrogen acquisition. However, exploring catalysts with suitable hydrogen binding strength for the HER process is always of great importance, but extremely challenging. In this work, sulfur and phosphor as electron-withdrawing elements were incorporated into carbon nanotube (CNT)-supported Ru catalysts, which were prepared through a facile solution reduction reaction and post thermo treatment. Owing to the suitable electronegativity provided by P and synergistic effects of the carbon nanotubes, the RuP 2 /CNT achieved a high catalytic performance as a HER electrocatalyst. This may result from the modulation effect of the electronic properties and the depressed adsorption free energy of RuP 2 . Electrochemical tests present that the RuP 2 /CNT composite exhibit a small overpotential of 58 mV at 10 mA cm −2 in acidic electrolyte. In a neutral or alkaline environment, the overpotential is 82 and 40 mV, respectively. The RuP 2 /CNT electrode also possesses stable durability for long-time cycling, suggesting its remarkable property as promising all-pH HER catalyst.
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JOURNAL OF THE ENERGY INSTITUTE
·
2019
·
IF 3.774
Biqin Lin,Rongxuan Li,Riyang Shu,Chao Wang,Zhengqiu Yuan,Yong Liu,Ying Chen
Hydrodeoxygenation (HDO) is an indispensable and important reaction in the fuel production process. Generally, the catalysts for HDO contain metal or acidic active sites, and the co-existence of them can significantly promote the HDO performance. While the subtle interaction between metal and acidic active sites is still not very clear. Herein, a series of Ru-based catalysts with different supports were prepared by photochemical method to obtain both of the high Ru dispersion and the moderate acidity. Among the catalysts with various supports, Ru/TiO 2 –Al 2 O 3 showed the most efficient performance in the HDO process of phenolic compounds. Guaiacol was converted into cyclohexane with above 90% selectivity at 240 °C. Other typical phenolic compounds, including phenol, anisole, p -cresol, 1,2-dimethoxybenzene, benzofuran , eugenol and dibenzyl ether, were all transformed into the corresponding cycloalkanes with yield close to 100%. The synergistic effect between highly dispersed Ru and moderate acid site played the key role for the enhanced production of hydrocarbon fuels. Moreover, this catalytic system was also effective on the raw bio-oil upgradation for producing high yield of hydrocarbons and alkylphenols, which has the potential to be used as biofuels.
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RSC Advances
·
2017
·Vol. 7
·期 80
·50634-50642
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IF 3.108
Lijun Luo,Libo Li,Xixi Xu,Dong Liu,Jinyang Li,Kun Wang,Tianyan You
Sensitive and quantitative analysis of pentachlorophenol (PCP) is especially important in the field of ecology and agriculture. Herein, a highly sensitive and stable Ru(bpy)32+-based anodic electrochemiluminescence (ECL) system utilizing nitrogen-doped graphene quantum dots (NGQDs) as a novel co-reactant was firstly constructed to detect PCP. In this system, Ru(bpy)32+ was used as luminophor, while NGQDs were applied as co-reactant in place of the toxic and volatile tripropylamine. The novel co-reactant not only promoted the luminous efficiency of Ru(bpy)32+, but also improved the stability of the ECL system. In addition, the enhancement mechanism of NGQDs on Ru(bpy)32+ and quenching mechanism of PCP on Ru(bpy)32+/NGQDs were investigated in detail. Under the optimum conditions, the as-fabricated sensor for ultrasensitive PCP determination expressed a wider linear range of 1 × 10−15 to 1 × 10−5 g mL−1 and a lower detection limit of 2 × 10−17 g mL−1 with good stability and repeatability. Furthermore, based on the distinctive advantages of the novel ECL sensor, it was successfully used to detect PCP in tap water and river water, and satisfactory recoveries were obtained.
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RSC Advances
·
2017
·Vol. 7
·期 81
·51452-51459
·
IF 3.108
Lihua Xie,Xiaoyan Wang,Fengli Yu,Bing Yuan,Congxia Xie,Shitao Yu
Amphiphilic mesoporous silica modified with trimethoxy (3,3,3-trifluoropropyl) silane (TFPS) and (3-aminopropyl) trimethoxysilane (APTS) was prepared by one-step synthesis. The structure and morphology of the mesoporous silica were characterized and confirmed by solid-state nuclear magnetic resonance, X-ray diffraction (XRD), N2 adsorption–desorption, Fourier transfer infrared spectroscopy (FT-IR), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Meanwhile, the thermostability of the amphiphilic mesoporous silica was detected by thermogravimetric (TG) technique. Highly dispersed Ru nanoparticles supported on such amphiphilic mesoporous silica (marked as Ru/MF@MN) were synthesized by wet impregnation method with the assistance of ultrasonic. The catalyst was characterized by X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma-atomic emission spectrometry (ICP-AES). In water medium, Ru/MF@MN was used in α-pinene hydrogenation to prepare cis-pinane. Under the optimum reaction conditions (35 °C, 2 MPa H2, 1 h, m (H2O) : m (α-pinene) : m (Ru/MF@MN) = 200 : 60 : 1), 99.9% α-pinene conversion and 98.9% cis-pinane selectivity were obtained. When Ru/MF@MN was recycled six times, the conversion slightly decreased and the selectivity was nearly unchanged.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Jingyi Yang,Yongzhen Gao,Jie Fan,Jieqiong Wang,Tao Yang,Zezheng Bing,Meng Zhang,Zhongyi Liu
Tuning the metal-support interaction (MSI) between highly dispersed nanosized metal particles and the support plays a pivotal role in the activity and selectivity of polyaromatics selective hydrogenation. In this work, the supported bimetallic Ni-Ru/SiO 2 -SEA catalyst was prepared by a strong electrostatic adsorption (SEA) strategy, and applied for the selective hydrogenation of biphenyl (BP) to cyclohexylbenzene (CHB). Compared to the catalysts prepared by the conventional incipient wetness impregnation method and Ni/SiO 2 -SEA, the significant effects of MSI and hydrogen spillover on Ni-Ru/SiO 2 -SEA facilitated the highly exposed and uniformly dispersed electron-deficient Ni δ+ (0 < δ < 2) species, which could enhance adsorption and activation of the electron-withdrawing phenyl group and H 2 , thereby promoting the efficient and selective conversion of BP to CHB. At the conditions of 160 ℃ and 2 MPa H 2 pressure, BP conversion over Ni-Ru/SiO 2 -SEA reached nearly 100 % within 3 h, achieving a remarkable selectivity of 97.9 % towards CHB, along with a high turnover frequency of 2756.9 h −1 for the active metallic Ni sites. Importantly, according to the kinetic simulations, the hydrogenation rate constant of Ni-Ru/SiO 2 -SEA was the highest (2.76 × 10 -2 mol·g −1 ·h −1 ) among the employed catalysts. Moreover, after six consecutive cycles, no obvious decline in hydrogenation efficiency was observed, confirming the remarkable activity and stability of Ni-Ru/SiO 2 -SEA. Furthermore, the activation of BP and desorption of CHB pathway on the Ni δ+ species were elaborated through temperature-programmed desorption characterization, highlighting the prominent contribution of MSI in enhancing the selective hydrogenation of polyaromatics.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yi Liu,Lianrui Cheng,Shuqing Zhou,Chenggong Niu,Tayirjan Taylor Isimjan,Xiulin Yang
Exploiting a cost-effective electrocatalyst for hydrogen oxidation reaction (HOR) with high-performance and CO poisoning resistance is essential for the widespread application of alkaline anion exchange membrane fuel cells (AEMFCs). Herein, we craft a unique Ru-RuP 2 heterostructure within hollow mesoporous carbon sphere (Ru-RuP 2 @C) using phosphide-controlled phase-transition approach. Benefiting from the interfacial electron transfer from RuP 2 to Ru, the Ru-RuP 2 @C electrocatalyst exhibits impressive HOR performance with a mass activity of 2.87 mA μ g Ru − 1 . Notably, Ru-RuP 2 @C demonstrates strong tolerance to 1000 ppm CO, a capability lacking in PtRu/C and Pt/C. When serves as an anode catalyst for AEMFC, it achieves a peak power density of 521 mW cm −2 , comparable to Pt/C. Experimental and theoretical analyses reveal that the built-in electric field, resulting from work function differences, creates an asymmetric charge distribution that modulates the d -band center of Ru-RuP 2 @C. This optimizes the adsorption strength of hydrogen and hydroxide intermediates, thereby accelerating HOR catalytic kinetics.
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