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1.
Nat Commun ; 15(1): 3100, 2024 Apr 10.
Artigo em Inglês | MEDLINE | ID: mdl-38600159

RESUMO

In heterogeneous catalysis catalyst activation is often observed during the reaction process, which is mostly attributed to the induction by reactants. In this work we report that surface structure of molybdenum nitride (MoNx) catalyst exhibits a high dependency on the partial pressure or concentration of reaction products i.e., CO and H2O in reverse water gas-shift reaction (RWGS) (CO2:H2 = 1:3) but not reactants of CO2 and H2. Molybdenum oxide (MoOx) overlayers formed by oxidation with H2O are observed at reaction pressure below 10 mbar or with low partial pressure of CO/H2O products, while CO-induced surface carbonization happens at reaction pressure above 100 mbar and with high partial pressure of CO/H2O products. The reaction products induce restructuring of MoNx surface into more active molybdenum carbide (MoCx) to increase the reaction rate and make for higher partial pressure CO, which in turn promote further surface carbonization of MoNx. We refer to this as the positive feedback between catalytic activity and catalyst activation in RWGS, which should be widely present in heterogeneous catalysis.

2.
Chemosphere ; 287(Pt 3): 132249, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34555584

RESUMO

Nano-zero-valent iron (nZVI), as a typical nano-material, has been recently used in wastewater treatment and combination with bioreactors. Using nZVI coupled denitrification system research the effect and influence of nZVI enhanced denitrification sludge on the degradation of toxic compounds and system performance. The nZVI coupled denitrification system showed better resistance to 2,6-DCP impact, and the concentrations of effluent NO2- and NO3- were below 2.0 mg/L. At the same time, the addition of nZVI enabled the denitrification system to quickly adapt to the toxic environment of 2,6-DCP within 15 days, and the degradation efficiency of 2,6-DCP reached 99.9%. The released SMP reduced after nZVI coupled with denitrification sludge in 2,6-DCP environment, which could improve the effluent water quality. Nuclear magnetic resonance spectroscopy showed that the addition of nZVI would change the structure of EPS in denitrification sludge. After 90 days of operation, the dominant bacteria in the denitrifying sludge have undergone great changes. Moreover, Thauera was responsible as the dominant bacteria for degrading 2,6-DCP in the denitrification system. The increased in the proportion of functional bacteria with nitrate_reduction, nitrogen_respiration, nitrate_respiration and nitrite_respiration in the presence of NZVI further reveals the mechanism of enhanced denitrification.


Assuntos
Desnitrificação , Nitratos , Clorofenóis , Ferro , Esgotos
3.
Adv Mater ; 31(41): e1903470, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31441152

RESUMO

Simultaneously achieving high Faradaic efficiency, current density, and stability at low overpotentials is essential for industrial applications of electrochemical CO2 reduction reaction (CO2 RR). However, great challenges still remain in this catalytic process. Herein, a synergistic catalysis strategy is presented to improve CO2 RR performance by anchoring Fe-N sites with cobalt phthalocyanine (denoted as CoPc©Fe-N-C). The potential window of CO Faradaic efficiency above 90% is significantly broadened from 0.18 V over Fe-N-C alone to 0.71 V over CoPc©Fe-N-C while the onset potential of CO2 RR over both catalysts is as low as -0.13 V versus reversible hydrogen electrode. What is more, the maximum CO current density is increased ten times with significantly enhanced stability. Density functional theory calculations suggest that anchored cobalt phthalocyanine promotes the CO desorption and suppresses the competitive hydrogen evolution reaction over Fe-N sites, while the *COOH formation remains almost unchanged, thus demonstrating unprecedented synergistic effect toward CO2 RR.

4.
Adv Sci (Weinh) ; 5(12): 1801216, 2018 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30581712

RESUMO

Nickel is regarded as the best alternative metal electrocatalyst to platinum for hydrogen evolution reaction (HER). Success in developing a quasi-amorphous metallic nickel (QAMN) nanopowder catalyst using a two-step chemical route for efficient and durable HER in alkaline solution is reported. It is found that the QAMN electrocatalyst exhibits essentially zero overpotential at the cathodic onset while delivering 10 mA cm-2 at an overpotential of only 240 mV; both performances are far better than what was reported previously using prior metallic nickel catalysts. Taking into account increased surface area, further enhanced activity is attributed to the superior intrinsic activity. Meanwhile, the QAMN catalyst shows excellent stability in accelerated and interrupted polarization in alkaline solution for tens of hours. This study provides a new chemical means to prepare amorphous metallic materials for more efficient catalysis.

5.
J Colloid Interface Sci ; 393: 58-65, 2013 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-23168043

RESUMO

Well-aligned CdS nanorod arrays (CdS NRs) with ~100 nm in diameter and ~700 nm in length were fabricated on FTO (fluorine-doped tin oxide) substrate by using glutathione as capping agents. The growth of CdS NRs was studied in details by exploring the roles of each active binding group in glutathione. The thiol group in glutathione plays an important role in forming a compact CdS nanocrystal film, upon which the nanorods grow subsequently via the synergetic effect of thiol and dicarboxyl groups in glutathione. The influence of surface passivation with glutathione on the photoelectrical property of CdS NRs was also tested. The results revealed that glutathione ligands encapsulated in the surfaces of CdS NRs act as insulating barriers between CdS NRs and solution, hindering charge transport. Hybrid photovoltaic cells of FTO/CdS NRs/P3HT (poly(3-hexylthiophene))/Au were then assembled. The performance of the photovoltaic devices was increased with increasing the length of the as-prepared CdS nanorods and further enhanced to the highest efficiency of 0.373% after the thermal sulfuration treatment.


Assuntos
Compostos de Cádmio/química , Técnicas Eletroquímicas , Glutationa/química , Nanotubos/química , Sulfetos/química , Tamanho da Partícula , Processos Fotoquímicos , Propriedades de Superfície
6.
Zhong Yao Cai ; 30(9): 1143-5, 2007 Sep.
Artigo em Chinês | MEDLINE | ID: mdl-18236762

RESUMO

OBJECTIVE: To study the extract process of Cyclic adenosinemonophosphate (cAMP) in Ziziphus jujuba. METHODS: CAMP was extracted with water, separated and purificated by ion exchange and silica gel G column chromatography. RESULTS: Thin layer chromatography (TLC) of the extracts and control cAMP showed the same Rf 0.75; The UV-absorption of the extracts and control cAMP had maximal absorb peak at 260 nm and the least absorb value at 230 nm; Infra-red spectrum of the extracts was indistinguishable from that of control cAMP; Retention time of the extracts by high-performance liquid chromatography (HPLC) determinate was 5.237 minute,unsettled impurity peak,content was 97%. Control cAMP was 5.350 minute,their retention time were of little difference. CONCLUSION: Chemistry structure of this extract with that of control cAMP is the same.


Assuntos
AMP Cíclico/isolamento & purificação , Frutas/química , Plantas Medicinais/química , Ziziphus/química , Cromatografia Líquida de Alta Pressão , AMP Cíclico/química , Géis , Resinas de Troca Iônica , Estrutura Molecular , Plantas Comestíveis/química , Tecnologia Farmacêutica/métodos
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