CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Miao Zhang,Limin Zhang,Mingrui Wang,Guanghui Zhang,Chunshan Song,Xinwen Guo
CO 2 hydrogenation to value-added light olefins (C 2–4 = ) is crucial for the utilization and cycling of global carbon resource. Moderate CO 2 activation and carbon chain growth ability are key factors for iron-based catalysts for efficient CO 2 conversion to target C 2–4 = products. The electronic interaction and confinement effect of electron-deficient graphene inner surface on the active phase are effective to improve surface chemical properties and enhance the catalytic performance. Here, we report a core-shell FeCo alloy catalyst with graphene layers confinement prepared by a simple sol-gel method. The electron transfer from Fe species to curved graphene inner surface modifies the surface electronic structure of the active phase χ-(Fe x Co 1– x ) 5 C 2 and improves CO 2 adsorption capacity, enhancing the efficient conversion of CO 2 and moderate C-C coupling. Therefore, the catalyst FeCoK@C exhibits C 2–4 = selectivity of 33.0% while maintaining high CO 2 conversion of 52.0%. The high stability without obvious deactivation for over 100 h and unprecedented C 2–4 = space time yield (STY) up to 52.9 mmol CO2 ·g –1 ·h –1 demonstrate its potential for practical application. This work provides an efficient strategy for the development of high-performance CO 2 hydrogenation catalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Bo Feng,Danning Feng,Yan Pei,Baoning Zong,Minghua Qiao,Wei Li
The photocatalytic oxidation of methane to methanol using molecule oxygen directly is an attractive catalytic reaction, but designing catalysts to avoid over-oxidation remains a significant challenge. Herein, Cu single-atom anchored on the defective carbon nitride structure (Cu SA/Def-CN) is designed for selective photocatalytic oxidation of methane into methanol using O 2 under mild conditions. The Cu SA/Def-CN catalyst exhibits a high methanol selectivity of 92.8% under optimized conditions. Mechanistic studies reveal a synergistic effect between Def-CN and Cu SA, where Def-CN is responsible for the in-situ generation of hydrogen peroxide, which is subsequently decomposed by the Cu SA sites to produce ·OH radicals that play a key role in the rate-determining step of methane activation to form methanol. Additionally, the presence of Cu SA not only enhances the electron-hole separation efficiency and improves the transfer of the photo-generated charges, but also increases the number of active sites for methane adsorption and activation. These insights provide valuable guidance for designing efficient catalysts for the highly selective photocatalytic oxidation of methane to methanol.
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NEW CARBON MATERIALS
·
2024
·
IF 6.5
Qing-shan Zhao,Qin-lian Liu,Yi-wen Li,Tian Ji,Yu-yue Yao,Yi-kun Zhao,Wei Deng,Han Hu,Ming-bo Wu
As by-products of petroleum refining, heavy oils are characterized by a high carbon content, low cost and great variability, making them competitive precursors for the anodes of potassium ion batteries (PIBs). However, the relationship between heavy oil composition and potassium storage performance remains unclear. Using heavy oils containing distinct chemical groups as the carbon source, namely fluid catalytic cracking slurry (FCCS), petroleum asphalt (PA) and deoiled asphalt (DOA), three carbon nanosheets (CNS) were prepared through a molten salt method, and used as the anodes for PIBs. The composition of the heavy oil determines the lamellar thicknesses, sp 3 -C/sp 2 -C ratio and defect concentration, thereby affecting the potassium storage performance. The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets (CNS-FCCS) that have a smaller layer thickness, larger interlayer spacing (0.372 nm), and increased number of folds than in CNS derived from the other three precursors. These features give it faster charge/ion transfer, more potassium storage sites and better reaction kinetics. CNS-FCCS has a remarkable K + storage capacity (248.7 mAh g −1 after 100 cycles at 0.1 A g −1 ), long cycle lifespan (190.8 mAh g −1 after 800 cycles at 1.0 A g −1 ) and excellent rate capability, ranking it among the best materials for this application. This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance, and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Zhenghao Mao,Wenjing Xu,Na Han,Yanguang Li
Aldehydes are valuable intermediates with widespread industrial applications, and their traditional synthesis relies on chemical oxidation that is often hazardous and environmentally unfriendly. Electrochemical oxidation offers a more sustainable and milder alternative; however, it faces challenges such as aldehyde overoxidation and susceptibility to base-catalyzed Cannizzaro disproportionation. Electrochemical glycerol oxidation to glyceraldehyde is a representative example, which typically requires precious metal-based electrocatalysts but still suffers from low selectivity and activity. Here, we report a metal-free oxidation strategy mediated by 2,2,6,6-tetramethylpiperidine-1-oxyl. By systematically investigating the redox thermodynamics and kinetics of TEMPO across a broad pH range, we construct a Pourbaix diagram and elucidate the relative kinetics of each reaction step. These insights allow us to explain the anomalously high apparent Faradaic efficiency (~200%) observed under acidic conditions, and identify neutral media as the optimal environment for selective glyceraldehyde production. Under optimized conditions, our system achieves a glyceraldehyde Faradaic efficiency exceeding 93% and a partial current density of 23.3 mA cm –2 at 0.57 V — more than doubling the performance of the best reported precious metal-based systems. Furthermore, the versatility of this strategy extends to the selective oxidation of other primary alcohols to their corresponding aldehydes with near-unity selectivity.
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Chinese Journal of Natural Medicines
·
2014
·
IF 0
De-Biao YAN,Dong-Ping ZHANG,Ming LI,Wen-Yuan LIU,Feng FENG,Bin DI,Qing-Long GUO,Ning XIE
To synthesize a series of 3-, 4-, and/or 11-trihydroxy modified bergenin derivatives and evaluated their cytotoxic activity in vitro . The phenolic hydroxyl groups of bergenin were protected by benzyl groups with benzyl bromide. Treatment of dibenzyl bergenin with the corresponding acid in the presence of EDC·HCl and DMAP in CH 2 Cl 2 , followed by hydrogenation over Pd/C catalysts, afforded derivatives of bergenin esters. All of the target compounds were identified by IR, MS, and 1 H NMR. Twenty-six novel and three known derivatives of bergenin esters were synthesized. Their cytotoxicity values were evaluated by the MTT assay on the inhibition of DU-145 and BGC-823 cells in vitro . Several triply-substituted ( 3a, 4a, 5a, 6a, 7a ) and doubly-substituted ( 8b, 9b ) bergenin derivatives exhibited higher cytotoxic activity than bergenin. The result showed that the size of substituents and the lipophilicity of the bergenin esters displayed an important role on their cytotoxic activity.
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PubMed
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
·
2014
·
IF 0.7
Yue XU,Chun-Jing TANG,Hong HUANG,Chao-Qun SUN,Ya-Kun ZHANG,Qun-Feng YE,Ai-Jun WANG
Fluorescent carbon quantum dots (CQDs) were synthesized by one-step hydrothermal treatment with apple juice as raw material. The result indicated that the fluorescence could be quenched by Hg 2+ with high specificity. Based on this phenomenon, a selective and sensitive sensor was constructed for the detection of Hg 2+ in phosphate solutions (pH 7.0). The fluorescence intensity showed linear responses with Hg 2+ concentration ranging from 5.0 to 100.0 nM and 1.0 to 50.0 μM, with the detection limit of 2.3 nM ( S / N = 3). The as-fabricated sensor was further extended for the determination of Hg 2+ in real water samples.
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CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Hao Wang,Xiaohao Liu,Guangyue Xu,Ziwei Guo,Ying Zhang
ABSTRACT Owing to Fe being the most abundant and least expensive transition metal on the earth, the utilization of Fe-based catalysts for catalytic hydrogenation has attracted worldwide attention. In this work, a series of N-doped C supported Fe catalysts (Fe-N-C) were prepared by co-pyrolysis of cellulose and ferric chloride under ammonia atmosphere. Characterization methods such as elemental analysis, atomic absorption spectroscopy, nitrogen adsorption-desorption isotherms, transmission electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were carried out to explore the physicochemical properties of the catalysts. Using hydrogenation of nitrobenzene as a model reaction, the catalysts prepared at different pyrolysis temperatures displayed different activities. Fe-N-C-700 exhibited the best activity among these catalysts, with the yield of aniline being up to 98.0% under 5 MPa H 2 at 120 °C after 12 h. Combined with the results of catalyst characterization and comparative tests, the transformation of Fe species and the generation of N-doped C, especially graphitized N-doped C, in the catalyst may be the main factors affecting the activity. A kinetic study was carried out and the apparent activation energy was obtained as 31.53 kJ/mol. The stability of the catalyst was also tested and no significant decrease in the activity was observed after 5 runs.
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CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Xiaona Liu,Yi Cao,Nana Yan,Chao Ma,Lei Cao,Peng Guo,Peng Tian,Zhongmin Liu
The high-temperature (HT) and low-temperature (LT) hydrothermal stabilities of molecular-sieve-based catalysts are important for the selective catalytic reduction of NO x with ammonia (NH 3 -SCR). In this paper, we report a catalyst, Cu 2+ loading SAPO-17, synthesized using cyclohexylamine (CHA), which is commercially available and inexpensive and is utilized in NH 3 -SCR reduction for the first time. After systematic investigations on the optimization of Si and Cu 2+ contents, it was concluded that Cu-SAPO-17-8.0%-0.22 displays favorable catalytic performance, even after being heated at 353 K for 24 h and at 973 K for 16 h. Moreover, the locations of CHAs, host–guest interaction and the Brönsted acid sites were explored by Rietveld refinement against powder X-ray diffraction data of as-made SAPO-17-8.0%. The refinement results showed that two CHAs exist within one eri cage and that the protonated CHA forms a hydrogen bond with O4, which indicates that the proton bonding with O4 will form the Brönsted acid site after the calcination .
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Wei Xiong,Min Zhou,Hao Li,Zhao Ding,Da Zhang,Yaokang Lv
ABSTRACT Owing to its cost-effectiveness and adjustable eight-electron distribution in the 3 d orbital, nickel oxide (NiO) is considered an effective electrocatalyst for an ambient electrochemical nitrogen reduction reaction (NRR). However, because of the low conductivity of the transition metal oxide electrocatalyst, its application in this field is limited. In this study, we found that the doping of NiO nanosheets with a small amount (3–10 nm) of Pt nanoparticles (Pt/NiO-NSs) leads to considerable improvements in the Faradaic efficiency (FE) and NH 3 yield compared with those obtained using pure NiO, breaking the common perception that commercial Pt-based electrocatalysts demonstrate little potential for NRR due to their high hydrogen evolution tendency. In a 0.1 mol/L Na 2 SO 4 solution at −0.2 V vs. RHE, a typical Pt/NiO-2 sample exhibits an optimum electrochemical NH 3 yield of 20.59 μg h –1 mg –1 cat. and an FE of 15.56%, which are approximately 5 and 3 times greater, respectively, than those of pure NiO nanosheets at the same applied potential. X-ray photoelectron spectroscopy analysis revealed that Pt in Pt/NiO-NSs exist as Pt 0 , Pt 2+ , and Pt 4+ and that high-valence Pt ions are more electropositive, thereby favoring chemisorption and the activation of N 2 molecules. Density function theory calculations showed that the d -band of Pt nanoparticles supported on NiO is significantly tuned compared to that of pure Pt, affording a more favorable electronic structure for NRR. The results of this study show that Pt can be an effective NRR electrochemical catalyst when loaded on an appropriate substrate. Most importantly, it provides a new synthetic avenue for the fabrication of highly active Pt-based NRR electrocatalysts.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2025
·
IF 4.7
Pan CHEN,Jia-yan LIU,Ji-hua ZHAI,Yao-hui YANG,Wei SUN
n-octylphosphonic acid (OPA) was introduced as a novel collector for ilmenite flotation and its effectiveness was compared with the conventional chelating collector, benzohydroxamic acid (BHA). Micro-flotation tests demonstrated that OPA was a highly effective and selective collector for separating ilmenite from titanaugite over acidic conditions (optimal pH around 3), which was also supported by adsorption amount measurements. X-ray photoelectron spectroscopy (XPS) tests indicated that the chemisorption of OPA onto ilmenite surface was much stronger than that of BHA. Solution chemistry diagram analyses indicated that OPA could dissociate well at pH 3.0 and mostly exist in anion form. DFT calculations further confirmed that OPA was much easier to adsorb onto ilmenite surface with shorter bond length and lower adsorption energy in comparison with BHA. Therefore, OPA maintained good collecting ability and selectivity for ilmenite flotation in the strongly acidic pulp, providing valuable insights into new collector design and development.
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NANOTECHNOLOGY
·
2012
·Vol. 23
·期 9
·095603
·
IF 3.979
Shaochun Tang,Sascha Vongehr,Xiangkang Meng
We report a general one-step route to place nanoparticles (NPs) of different noble metals controllably into interior or surface locations of submicron nanoporous carbon spheres (CSs). In particular, Pd and Au NPs can be easily put either inside or outside of the CSs by selecting these metals' differently charged precursor ions. Employing mixed precursor solutions, the method allows different metals to grow simultaneously yet selectively in the separate locations, thus resulting in composites with a complex layered structure, for example Pd or Au outside and Ag inside, Au or Pt outside and Pd inside, and other combinations. The synthesis is fast and needs no additional steps like a functionalization of surfaces. It crucially involves microwave heating, the power setting of which further influences the locations and sizes of the NPs especially in the interior of the amorphous carbon matrix. The three-dimensional composite structures are analyzed by transmission electron microscopy and energy dispersed x-ray spectroscopy combined with quantitative analysis by comparison with simulation. The UV–visible absorption of monometallic and layered composites is compared. The involved mechanisms leading to the selective decoration are discussed; important aspects being the charge of the precursor ions and selective microwave absorption.
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JOURNAL OF RARE EARTHS
·
2017
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IF 2.429
Yanran XUN,Xinxin HE,Han YAN,Ziwang GAO,Zhao JIN,Chunjiang JIA
In this paper, a series of Fe- and Co-doped lanthanum (hydr)oxides catalysts were prepared by a simple coprecipitation-hydrothermal method. The as-prepared catalysts were characterized with various techniques including powder X-ray diffraction (XRD), N 2 adsorption/desorption, inductively coupled plasma (ICP) and transmission electron microscopy (TEM). The Fe-based catalysts exhibited consecutive phase changes of amorphous FeO x →FeLaO 3 →Fe 2 N under different stages (as-prepared→calcination→ammonia decomposition reaction); as for Co-based catalysts, the phase transformation followed a sequence of Co(OH) 2 → Co 3 O 4 →metallic Co. It was revealed that Fe 2 N and metallic Co were most probably the active crystalline phase respectively for Fe- and Co-based catalysts in the decomposition of ammonia.
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