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Catalysts · 2022 ·Vol. 12 ·期 12 ·1515 · IF 4.501

Cu/CuOx@C Composite as a High-Efficiency Electrocatalyst for Oxygen Reduction Reactions

Ding Zhang,Yun-Fei Li,Li-Xue Liu,Lei Duan,Zhi-Li Ren,Shou-Dong Xu,Liang Chen,Hui-Juan Guo,Yi Huang,Li-Juan Shi,Qun Yi

Among clean energy transformation devices, fuel cells have gained special attention over the past years; however, advancing appropriate non-valuable metal impetuses to halfway supplant the customary Pt/C impetus is still in progress. In this paper, we propose a specific electrocatalyst in the formula of highly-active Cu species, associated with coated carbon (Cu@C-800), for oxygen reduction reaction (ORR) through post-treatment of a self-assembled precursor. The optimized catalyst Cu@C-800 showed excellent ORR performance (i.e., the onset potential was 1.00 V vs. RHE, and half-wave potential of 0.81 V vs. RHE), high stability, resistance to methanol, and high four-electron selectivity. The enhancement is attributed to the synergy between the carbon matrix and a high explicit surface region and rich Cu nano-species.

研究领域: 材料科学 · 能源化学
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International Journal of Minerals Metallurgy and Materials · 2024 ·Vol. 31 ·期 3 ·552-561 · IF 5.6

Constructing Al@C–Sn pellet anode without passivation layer for lithium-ion battery

Cao Kangzhe,Wang Sitian,He Yanan,Ma Jiahui,Yue Ziwei,Liu Huiqiao

Al is considered as a promising lithium-ion battery (LIBs) anode materials owing to its high theoretical capacity and appropriate lithation/de-lithation potential. Unfortunately, its inevitable volume expansion causes the electrode structure instability, leading to poor cyclic stability. What’s worse, the natural Al 2 O 3 layer on commercial Al pellets is always existed as a robust insulating barrier for electrons, which brings the voltage dip and results in low reversible capacity. Herein, this work synthesized core–shell Al@C–Sn pellets for LIBs by a plus-minus strategy. In this proposal, the natural Al 2 O 3 passivation layer is eliminated when annealing the pre-introduced SnCl 2 , meanwhile, polydopamine-derived carbon is introduced as dual functional shell to liberate the fresh Al core from re-oxidization and alleviate the volume swellings. Benefiting from the addition of C–Sn shell and the elimination of the Al 2 O 3 passivation layer, the as-prepared Al@C–Sn pellet electrode exhibits little voltage dip and delivers a reversible capacity of 1018.7 mAh·g −1 at 0.1 A·g −1 and 295.0 mAh·g −1 at 2.0 A·g −1 (after 1000 cycles), respectively. Moreover, its diffusion-controlled capacity is muchly improved compared to those of its counterparts, confirming the well-designed nanostructure contributes to the rapid Li-ion diffusion and further enhances the lithium storage activity.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米结构设计 · 金属基复合材料
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Constructing Robust Cathode/Electrolyte Interphase for Ultrastable 4.6 V LiCoO2 under −25 °C

Bin Ye,Mingzhi Cai,Miao Xie,Hang Dong,Wujie Dong,Fuqiang Huang

Improving the durability of cathode materials at low temperature is of great importance for the development nowadays of lithium ion batteries, since the practical capacity and cycling stability of the electrode are reduced significantly at low temperature. Herein, by amorphous Zr3(PO4)4 surface engineering, we realize a stable high-voltage LiCoO2 operation (4.6 V) at −25 °C. The highly amorphous surface layer can help to form a high-quality cathode-electrolyte interphase with strong stability and low interface resistance, especially at low temperature. Such a surface-engineered LiCoO2 shows a capacity of 179.2 mAh g–1 at 0.2C and an excellent cyclability with 91% capacity retention after 300 cycles (1C). As a comparison, bare LiCoO2 shows only 161.6 mAh g–1 and 1% capacity retention under the same circumstances. This work confirms that surface regulation and control engineering is an effective route to improve the high-voltage and low-temperature performance of LiCoO2.

研究领域: 材料科学 · 电化学 · 储能技术 · 表面工程 · 电池技术
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SOLID STATE IONICS · 2023 · IF 3.2

A novel double-coated anode material SiOx/C/Cu2O for lithium ion batteries

Jizhe Wu,Chenxin Jin,Guojun Xu,Huaide Chen,Bin Lu,Xiaomin Li,Fugen Sun,Lang Zhou,Zhihao Yue

Silicon monoxide (SiO x , 0 < x < 2) has been one of the new directions of scientific researchers because of some characteristics, such as higher theoretical specific capacity and lower volume expansion efficiency. However, its disadvantages such as the volume expansion effect and poor conductivity still exist in the process of charge and discharge, which limit its commercialization process. In this paper, cuprous oxide and carbon coated silicon monoxide (SiO x /C/Cu 2 O) composites were obtained by high temperature heat treatment. In the SiO x /C/Cu 2 O anodes, carbon can buffer the volume expansion of the lithium intercalation, enhance the conductivity of the material, reduce the contact between the electrolyte and the active substance, Cu 2 O can further reduce the contact between the electrolyte and the active substance, greatly buffer the change of electrode structure and improve the overall cycling performance. After the rate of 0.5C (1C = 2100 mA g −1 ) for 500 cycles, the discharge specific capacity is 704.0 mAh g −1 , about 350 mAh g −1 higher than SiO x , which shows excellent long-cycle ultra-high stability.

CAS / MDL: 9003-35-4
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INORGANIC CHEMISTRY COMMUNICATIONS · 2023 · IF 3.8

Thermal physical and magnetic properties of water-based yolk-shell Fe3O4@C nanofluids

Zichang Shi,Shan Qing,Zhumei Luo,Yiqin Liu,Jiachen Li

Fe 3 O 4 @C yolk-shell nanoparticles were synthesized by a one-pot solvothermal method using ferrocene as raw material and dispersed in deionized water to configure four different concentrations of water-based Fe 3 O 4 @C nanofluids. The morphology of Fe 3 O 4 @C nanoparticles was characterized. The results showed that the average particle size of Fe 3 O 4 @C nanoparticles was in the range of 82–84 nm with stable yolk-shell structure and large specific surface area. The stability of Fe 3 O 4 @C nanofluid was investigated. The results showed that Fe 3 O 4 @C nanofluid has good stability with maximum zeta potential values at pH 8–9. The thermal properties of Fe 3 O 4 @C nanofluids were investigated, and for the prepared nanofluids, the thermal conductivity increased with temperature and nanoparticle concentration, possessing excellent thermal stability. The magnetic responsiveness of Fe 3 O 4 @C nanofluid was characterized, and the results showed that the magnetic properties of Fe 3 O 4 @C nanofluid increased with increasing concentration.

CAS / MDL: 102-54-5
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TALANTA · 2023 · IF 6.1

A facile indole probe for ultrasensitive immunosensor fabrication toward C-reactive protein sensing

Yun-Yun Cheng,Xiao-Zhen Feng,Tao Zhan,Qi-Qi An,Guo-Cheng Han,Zhencheng Chen,Heinz-Bernhard Kraatz

C-reactive protein (CRP) is a protein biomarker for acute phase response. Herein, we fabricate a highly sensitive electrochemical immunosensor for CRP on a screen-printed carbon electrode (SPCE) with indole as a novel electrochemical probe and Au nanoparticles for signal amplification. Amongst, indole appeared as transparent nanofilms on the electrode surface, and underwent a one-electron and one-proton transfer to form oxindole during the oxidation process. Upon optimization of experimental conditions, a logarithmic correlation between CRP concentration (0.0001–100 μg∙mL −1 ) and response current was revealed with a detection limit of 0.03 ng∙mL −1 and a sensitivity of 5.7055 μA∙μg −1 ∙mL∙cm −2 . The sensor exhibited exceptionally distinction selectivity, reproducibility and stability of the electrochemical immunosensor studied. The recovery rate of CRP in human serum samples determined by the standard addition method, ranged between 98.2–102.2%. Overall, the developed immunosensor is promising, and has the potential for CRP detection in real human serum samples.

CAS / MDL: 9048-46-8 70024-90-7
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Carbon Energy · 2023 ·Vol. 5 ·期 9 ·e339 · IF 20.5

Noncovalent interactions on the electrocatalytic oxidation of ethanol on a Pt/C electrocatalyst

Chenjie Han,Yeqing Lyu,Shaona Wang,Biao Liu,Yi Zhang,Jun Lu,Hao Du

Due to their environmentally friendly nature and high energy density, direct ethanol fuel cells have attracted extensive research attention in recent decades. However, the actual Faraday efficiency of the ethanol oxidation reaction (EOR) is much lower than its theoretical value and the reaction kinetics of the EOR is sluggish due to insufficient active sites on the electrocatalyst surface. Pt/C is recognized as one of the most promising electrocatalysts for the EOR. Thus, the microscopic interfacial reaction mechanisms of the EOR on Pt/C were systematically studied in this work. In metal hydroxide solutions, hydrated alkali cations were found to bind with OH ad through noncovalent interactions to form clusters and occupy the active sites on the Pt/C electrocatalyst surface, thus resulting in low Faraday efficiency and sluggish kinetics of the EOR. To reduce the negative effect of the noncovalent interactions on the EOR, a shield was made on the electrocatalyst surface using 4-trifluoromethylphenyl, resulting in twice the EOR catalytic reactivity of Pt/C.

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Catalysis Science & Technology · 2023 ·Vol. 13 ·期 6 ·1855-1865 · IF 5

Photocatalytic C–N coupling towards urea synthesis with a palladium-supported CeO2 catalyst

Shuyi Yang,Jiayi Deng,Jiaying Chen,Qingmei Tan,Tianren Liu,Ke Chen,Dongxue Han,Yingming Ma,Mengjiao Dai,Li Niu

The conversion of N2 and CO2 into urea through a photocatalytic C–N coupling reaction under ambient conditions serves as a novel green avenue for urea synthesis. However, the poor adsorption and C–N coupling capability of inert gas molecules hinder the efficient catalytic activity. Herein, palladium-decorated CeO2 (Pd–CeO2) was demonstrated as an efficient photocatalyst for C–N coupling reaction and delivered a remarkable urea yield rate of 9.2 μmol h−1 g−1, which was superior to that of pristine CeO2 (2.5 μmol h−1 g−1). Comprehensive investigations further endorsed that the emerged space-charge region in the CeO2(111)/Pd(111) interface not only effectively facilitates the targeted capture and activation of inert CO2 and N2 but also stabilizes the formation of key intermediates (*NCON). Besides, the effective inhibition of the endothermic *NNH intermediate is conducive to the subsequent C–N coupling process and the improvement of reaction selectivity. The reaction mechanism was studied in detail by density functional theory (DFT) with the formation of a C–N bond via a thermodynamically spontaneous reaction between *NN* and CO. This work provides novel insights into the conversion of CO2 and N2 into urea.

CAS / MDL: 7803-57-8
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CRYSTENGCOMM · 2023 ·Vol. 25 ·期 6 ·981-987 · IF 3.1

Anchored RuSe2 nanospheres on Co–N–C nanosheets boost electrocatalytic alkaline hydrogen evolution

Nan Li,Minghao Shi,Wei Zhan,Wenjing Shen,Mianmian Wu,Guifang Sun,Qingfei Li,Jiangquan Ma

Ru-based catalysts are potential substitutes for Pt in the hydrogen evolution reaction (HER). It is worth noting that the Se ions in RuSe2 can modulate the electronic structure of the Ru metal, thus effectively improving the HER kinetics of RuSe2. However, single electronic structure modulation is hard to complete due to the electron deficiency of active Ru atoms. Herein, we prepare and design a novel RuSe2/Co–N–C (RuSe2 nanospheres supported on Co–N–C nanosheets) electrocatalyst with two-electron modulation by a hydrothermal and thermal annealing method. Benefiting from the uniform distribution of RuSe2 nanospheres on Co–N–C nanosheets and Co–N–C nanosheets acting as additional electron donors to make up for the electron deficiency of the Ru metal, RuSe2/Co–N–C exhibits excellent HER performance with a low overpotential of 26.4 mV at 10 mA cm−2 and a low Tafel slope of 53.2 mV dec−1. This work offers an effective method for the synthesis of high catalytic performance electrocatalysts by constructing an interaction between the carrier and the active metal.

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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES · 2023 ·Vol. 24 ·期 2 ·1454 · IF 5.6

Identification of Human UDP-Glucuronosyltransferase Involved in Gypensapogenin C Glucuronidation and Species Differences

Juan Chen,Lin Qin,Xingdong Wu,Daopeng Tan,Yanliu Lu,Yimei Du,Di Wu,Yuqi He

Gypensapogenin C (GPC) is one of the important aglycones ofGynostemma pentaphyllum(GP), which is structurally glucuronidated and is highly likely to bind to UGT enzymes in vivo. Due to the important role of glucuronidation in the metabolism of GPC, the UDP-glucuronosyltransferase metabolic pathway of GPC in human and other species’ liver microsomes is investigated in this study. In the present study, metabolites were detected using high-performance liquid chromatography–tandem mass spectrometry (LC–MS/MS). The results show that GPC could generate a metabolite through glucuronidation in the human liver microsomes (HLMs). Additionally, chemical inhibitors combined with recombinant human UGT enzymes clarified that UGT1A4 is the primary metabolic enzyme for GPC glucuronidation in HLMs according to the kinetic analysis of the enzyme. Metabolic differential analysis in seven other species indicated that rats exhibited the most similar metabolic rate to that of humans. In conclusion, UGT1A4 is a major enzyme responsible for the glucuronidation of GPC in HLMs, and rats may be an appropriate animal model to evaluate the GPC metabolism.Keywords:gypensapogenin C;glucuronidation;human liver microsomes;UGT1A4;species differences

CAS / MDL: 27061-78-5 7791-18-6
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International Journal of Electrochemical Science · 2023 · IF 1.5

Synthesis of Highly Active Pt-Pd-Cu/C Catalysts for Formic Acid Oxidation

Yange Suo,Yuxin Guo,Chenbin Rong,Zhiguo Zhang,Guilin Hu

This work reports the synthesis of a series of carbon supported Pt-Pd-Cu (Pt-Pd-Cu/C) nano-catalysts for formic acid oxidation. The trimetallic catalysts were prepared by a one-pot protocol through reduction of Pt, Pd and Cu ions using ethylene glycol and sodium citrate as the reducing and stabilizing reagents. XRD characterization suggests that Pt-Pd-Cu alloys with different lattice parameters can be successfully prepared through adjusting the atomic ratios of Pt, Pd and Cu ions in the precursor solutions. The average crystal sizes of the Pt-Pd-Cu/C catalysts are in the range of 2.7-3.1 nm. TEM images shows that the metallic nanoparticles are well dispersed on the carbon surface, with Pt 1 Pd 3 Cu 3 /C catalyst showing obvious aggregation. XPS was carried out to analyze the surface compositions, as well as the chemical states of the novel metals in the catalysts. The real atomic ratios of the metals in the catalysts based on ICP-OES evaluation are consistent with the stoichiometric values. Electrochemical analysis suggests that the activities the Pt-Pd-Cu/C catalysts towards formic acid oxidation are dependent on the composition of the catalysts, with Pt 1 Pd 4 Cu 2 /C exhibiting the best performance. A mass normalized peak current density of 3.02 A/mg (Pt+Pd) was observed on Pt 1 Pd 4 Cu 2 /C catalyst.

CAS / MDL: 13820-40-1 64-18-6
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Catalysis Science & Technology · 2023 ·Vol. 13 ·期 15 ·4489-4497 · IF 5

Ceria crystal facet impact for methane C–H activation in Pd/CeO2 catalysts

Kewu Yang,Ke Wang,Xianfeng Shen,Fanxing Zhang,Bei Huang,Keping Yan,Yao Shi,Yi He,Pengfei Xie

The exposed facets of ceria crystals have a profound effect on the reactivity of ceria-supported catalysts owing to the intricate metal–support interactions. In this work, ceria nanorods, nanocubes, and polyhedra, with corresponding exposed (110)/(100), (100), and (111) terminations, were hydrothermally synthesized to support Pd species, with the aim of investigating the in-depth impacts of ceria crystal facets for methane combustion over ceria-supported palladium catalysts. The nanorod sample delivered the highest methane conversion (T50 = 277 °C, GHSV = 200 000 mL h−1 gcat−1) and greater reaction rate (9.59 × 10−4 molCH4 h−1 gcat−1), 1.23 times that of nanocubes and 3.14 times that of polyhedra. Further characterizations revealed that on the (110)/(100) surface planes, PdOx exhibited stronger interactions with CeO2. This led to enhanced formation of Pd4+ and higher reducibility of PdOx species, thus promoting methane activation. This work would supply experimental insights into the relationship between exposed facets and reactivity, as well as guidance for rational catalyst design.

CAS / MDL: 10294-41-4 10102-05-3
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