ACS Applied Energy Materials
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2019
·
IF 0
Li-Ping Yang,Jian-Li Mi,Jia-Hao Liang,Zhao-Yang Zu,Peng Zhang
A simple and efficient method was developed to prepare a copper–carbon (Cu–C) catalyst with high oxygen reduction reaction (ORR) activity via direct pyrolysis of a mixture of metal salts (Cu(NO3)2·3H2O and Zn(CH3COO)2) and 1,3,5-benzenetricarbocylic acid at 1010 °C under a N2 stream. It is found that the Cu–C catalyst exhibits superior catalytic activity toward ORR with a half-wave potential of 0.81 V and a four-electron transfer pathway in 0.1 M KOH electrolyte. Generally, it is known that N plays an important role for the high ORR catalytic activities of nonprecious metal-doped carbon materials. Herein, we demonstrate that N is not required for the superior catalytic activity of Cu–C materials. Both the Cu particles and the embedded Cu atoms in the carbon substrate are suggested to provide the ORR active sites. In addition, despite the fact that the Zn is removed during the pyrolysis, the adding of Zn salt in the precursor is important for the enhanced catalytic activity. The evaporation of Zn during the pyrolysis results in the large surface area of the catalyst, which is beneficial to the mass transfer during the catalytic process. Moreover, a large number of carbon defects can be created via the removal of Zn atoms that facilitated the ORR.
研究领域:
材料科学
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电化学
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催化
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DOI
ACS Applied Nano Materials
·
2023
·
IF 5.9
Hua Li,Mudong Tu,Yahan Fang,Tianzhi Hao,Baodui Wang
At present, a variety of catalysts have been studied and used for the electrocatalytic reduction of nitrate. However, it is still a great challenge to improve the selectivity of the electrocatalytic nitrate reduction reaction (NO3–RR) catalyst for ammonia and reduce the activity of the competitive reaction. Herein, two-dimensional CuOx nanosheets with abundant oxygen vacancy defects were in situ grown on Cu nanoparticles to construct Cu/2D-CuOx composite nanomaterials as nitrate reduction electrocatalysts. The two-dimensional (2D) nanosheet morphology facilitated the exposure of active sites and promoted the mass/charge transfer process during electrocatalysis. As a result, the synergistic effect of abundant oxygen vacancy defects and the 2D nanosheet-like structure on the surface of the catalyst endows the Cu/2D-CuOx with superior performance for the nitrate reduction reaction, achieving high ammonia selectivity (97.56%) and NH4+ yield (1476 μg h–1 mg–1).
研究领域:
材料科学
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电化学
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催化
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环境化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Liye Shuai,Qun Li,Jia Liu,Jiabin Wu,Xinning Huang,Jianglong Yu,Jinxiao Dou,Huaiguang Li,Xingxing Chen
The rational design of efficient photoanodes is essential for advancing solar-driven water oxidation. This study addresses the intrinsic challenges of bismuth vanadate (BiVO 4 ), such as sluggish charge kinetics and severe surface recombination, through the construction of a ternary composite photoanode via synergistic interfacial modification and cocatalyst integration. A hierarchical architecture was fabricated through sequential low-temperature chemical bath deposition and electrodeposition, integrating a CoFe-layered double hydroxide (CoFe-LDH) interlayer and nickel-hydroxynitrate (Ni 2 (NO 3 ) 2 (OH) 2 ) onto BiVO 4 substrates. The optimized BiVO 4 /CoFe-LDH@Ni 2 (NO 3 ) 2 (OH) 2 photoanode achieves a photocurrent density of 5.57 mA/cm 2 at 1.23 V vs. reversible hydrogen electrode (V RHE ) under Air Mass 1.5 Global (AM 1.5G) illumination, accompanied by a 251 mV cathodic shift in onset potential. Comprehensive characterizations-including X-ray photoelectron spectroscopy (XPS), open-circuit photovoltage (OCP) decay, time-resolved photoluminescence (TRPL) decay, electron paramagnetic resonance (EPR) and Kelvin probe force microscopy (KPFM)-reveal that the oxygen vacancy (O v )-rich CoFe-LDH@Ni 2 (NO 3 ) 2 (OH) 2 layer facilitates efficient charge transfer within BiVO 4 and generates a pronounced built-in electric field, thereby significantly enhancing interfacial charge separation. Concurrently, density functional theory (DFT) calculations demonstrate that the interfacial effect of CoFe-LDH@Ni 2 (NO 3 ) 2 (OH) 2 substantially lowers the thermodynamic barrier for the oxygen evolution reaction (OER). This study offers fundamental insights for fabricating high-efficiency BiVO 4 -based photoanodes.
研究领域:
材料科学
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物理化学
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能源化学
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光催化
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半导体电化学
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DOI
高影响因子
SYNTHESIS-STUTTGART
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2019
·Vol. 51
·期 17
·3221-3230
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IF 2.867
Wei Sun,Mingjuan Zhang,Peilang Li,Yiqun Li
A novel and highly efficient one-pot synthesis of polysubstituted imidazoles from α-hydroxyphenylacetic acids, diphenylacetylene, and amines has been achieved by Pd(OAc)2/Ce(SO4)2/Bi(NO3)3 trimetallic catalytic system. A series of control experiments showed that this overall reaction occurs through a one-pot cascade process combining the steps of decarboxylation of α-hydroxyphenylacetic acids, Wacker-type oxidation of diphenylacetylene, and Debus–Radziszewski annulation of aryl aldehydes and benzil generated in situ, as well as amines. This reaction represents a novel multicomponent reaction using α-hydroxyphenylacetic acids and diphenylacetylene as sources of aryl aldehydes and a β-diketone. This process exhibits a broad substrate scope and a good functional group tolerance to assemble the corresponding polysubstituted imidazoles in excellent yields (72–88%) under mild conditions.
研究领域:
有机化学
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催化化学
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药物化学
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合成方法学
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杂环化学
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DOI
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
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2021
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IF 3.178
Yaqi Ding,Neng Gao,Nian Li,Guangming Chen,Yongmei Xuan
The vapour-liquid equilibrium (VLE) data of four ternary solutions HCOOK + [Emim]Ac /[Emim]Br / [Emim]Cl / [Emim]NO 3 + H 2 O were measured using the boiling method at the temperatures from 305.78 K to 387.08 K, at solute (HCOOK + IL) mass fractions ( w ) between 0.2 and 0.5. A total of 234 data points ( w = 0 included) were obtained and correlated with empirical Antoine-type equations. The absolute average relative deviations (AARD %) between calculated and measured vapour pressures were 0.58%, 0.50%, 0.49%, 0.63%, respectively, which showed good agreement. The comparison of the experimental and standard data and combined uncertainties of the experimental data confirmed good reliability of the experimental method and apparatus. The four ternary solutions with ILs as additives have lower vapour pressure compared to the corresponding binary solutions without ILs. The results showed that the four ternary solutions of HCOOK + [Emim]Ac / [Emim]Br / [Emim]Cl / [Emim]NO 3 + H 2 O can be the alternatives for traditional dehumidification and absorption media. [Emim]Cl has the best ability to reduce the vapour pressure of HCOOK + H 2 O at the solute (HCOOK + IL) mass fraction of 0.4 and 0.5. The [Emim]Ac has the most effect reducing the vapour pressure of HCOOK + H 2 O at the solute (HCOOK + IL) mass fraction of 0.3.
研究领域:
化学工程
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热力学
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DOI
高影响因子
DALTON TRANSACTIONS
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2022
·Vol. 51
·期 39
·15111-15120
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IF 4.569
Jiao Wang,Linlin Zhang,Yuanyuan Wang,Yongjian Niu,Dong Fang,Qingxiao Su,Cheng Wang
Electrocatalytic nitrate reduction offers a sustainable route to ammonia synthesis and wastewater treatment. However, the nitrate-to-ammonia conversion remains inefficient due to the sluggish kinetics and diverse side reactions. Herein, well-faceted CuNi nanocrystals with Ni-rich surfaces and favorable d-band centres were synthesized with the assistance of γ-cyclodextrin via a solvothermal process. When used as catalysts for nitrate electroreduction, they delivered an ammonia yield of 1.374 mmol h−1 mg−1 (0.5496 mmol h−1 cm−2) at −0.3 V with the faradaic efficiency and selectivity reaching 94.5% and 65.0%, respectively, surpassing pure Cu or Ni nanocrystals and most reported catalysts. Such excellent performances originated from the optimal geometric and electronic structures and special element distribution, which optimized the adsorption behaviors and accelerated the reaction kinetics. A NO3−–NO2−–NH3 pathway was proposed with the chemical process following the initial electron transfer process as the rate-determining step. This work sheds light on the design of efficient catalysts to achieve carbon neutrality through simultaneous geometric and electronic structure modulation.
研究领域:
材料科学
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催化
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环境化学
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电化学
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DOI
PubMed
高影响因子
Sustainable Energy & Fuels
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2020
·Vol. 4
·期 4
·1780-1788
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IF 5.503
Jing Wang,Jing Li,Meiri Wang,Yuanyuan Liu,Hongtao Cui
Battery-type electrode materials such as Ni(OH)2 applied in Faraday supercapacitors could present a low cycling stability due to the microstructure damage of materials, originating from their cyclic volume swelling and shrinking. It is well established that the structural stability of materials is crucial for their cycling stability. However, the lack of knowledge about the structural relevance of materials to their cycling stability somehow results in a chaotic understanding on the material design. In this study, we try to reveal the structural relevance by comparing an orderly built nanostructure with a randomly packed nanostructure using Ni(OH)2 as the target material. It is found that the branched nanosheet-interlaced nanostructure of Ni(OH)2 has its self-supportive function in favor of its structural stability, thus promoting its cycling stability. Also, the orderly nanostructured Ni(OH)2 presents high electrochemical performance due to the reduced interfacial charge-transfer resistance and Warburg resistance.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rongwei Zhong,Hu Li,Yangyang Wang,Ying Zhang,Jian Zhou,Tiecheng Wang
Municipal wastewater treatment plants (MWTP) are the main gathering places for antibiotic resistance genes (ARGs) and pathogenic bacteria. In this study, plasma oxidation was applied to remove the ARGs and inhibit pathogenicity in the effluent. The experimental results demonstrated that approximately 1.32 log, 1.34 log, 2.39 log, and 2.80 log of aac (3)-II , bla TEM-1 , Tet W, and Tet C were removed within 25 min of the plasma treatment, respectively. OH, 1 O 2 , O 3 , H 2 O 2 , NO 2 − , and NO 3 − all contributed to ARG removal. Coexisting dissolved organic matter was also oxidized, which was positively related to ARG removal. Plasma oxidation led to a decrease in the diversity and richness of microbial communities; Parcubacteria and Proteobacteria were the main potential hosts of ARGs and mobile genetic elements. Integron gene IntI 1 decreased by 2.46 log after plasma treatment, which was positively related to ARG removal. Gene expression related to ATP binding, DNA repair, gene transfer, and the cell membrane was reduced after plasma treatment, resulting in effective ARG removal. Furthermore, pathogenic genes related to lumpy skin disease, Niemann-Pick disease, polycystic kidney and hepatic disease were all down-regulated by plasma treatment. Overall, the plasma treatment inhibited the transmission risks of ARGs and pathogenicity in the effluent of MWTP.
研究领域:
环境科学
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微生物学
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水处理
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生物技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）