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1.
Small ; : e2401872, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38639027

RESUMO

Electrochemical glycerol oxidation features an attractive approach of converting bulk chemicals into high-value products such as glyceric acid. Nonetheless, to date, the major product selectivity has mostly been limited as low-value C1 products such as formate, CO, and CO2, due to the fast cleavage of carbon-carbon (C-C) bonds during electro-oxidation. Herein, the study develops an atomically ordered Ni3Sn intermetallic compound catalyst, in which Sn atoms with low carbon-binding and high oxygen-binding capability allow to tune the adsorption of glycerol oxidation intermediates from multi-valent carbon binding to mono-valent carbon binding, as well as enhance *OH binding and subsequent nucleophilic attack. The Ni3Sn electrocatalyst exhibits one of the highest glycerol-to-glyceric acid performances, including a high glycerol conversion rate (1199 µmol h-1) and glyceric acid selectivity (62 ± 3%), a long electrochemical stability of > 150 h, and the capability of direct conversion of crude glycerol (85% purity) into glyceric acid. The work features the rational design of highly ordered catalytic sites for tailoring intermediate binding and reaction pathways, thereby facilitating the efficient production of high-value chemical products.

2.
J Food Sci ; 88(7): 3102-3118, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37219382

RESUMO

In this study, male mice were treated with fermented and unfermented Lactobacillus plantarum, Lactobacillus bulgaricus, and Lactobacillus rhamnosus black wolfberry juice (10 mL/kg/day) for 40 days, and their prophylactic effects on ulcerative colitis (UC) induced by dextran sodium sulfate were investigated. The intervention of black wolfberry juice reduced the levels of pro-inflammatory cytokines and increased the content of anti-inflammatory cytokines in the serum and colon. In addition, the pathological changes in colon tissue were alleviated, the expression of Bcl-2 protein in the colon was enhanced, and the intestinal microbiota of the mice was regulated, with an increase in Bacteroidetes and a decrease in Helicobacter. These results suggested that black wolfberry juice had an anti-UC function and Lactobacillus fermentation enhanced the anti-inflammatory effect of black wolfberry juice by modulating the intestinal microbiota.


Assuntos
Colite Ulcerativa , Colite , Lycium , Probióticos , Masculino , Animais , Camundongos , Colite Ulcerativa/induzido quimicamente , Colite Ulcerativa/tratamento farmacológico , Colite Ulcerativa/prevenção & controle , Sulfato de Dextrana/efeitos adversos , Lactobacillus/metabolismo , Colo/metabolismo , Anti-Inflamatórios/farmacologia , Citocinas/metabolismo , Probióticos/uso terapêutico , Modelos Animais de Doenças , Camundongos Endogâmicos C57BL , Colite/induzido quimicamente
3.
Sci Bull (Beijing) ; 67(10): 1042-1048, 2022 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-36546248

RESUMO

Although many catalysts have been reported for the CO2 electroreduction to C1 or C2 chemicals, the insufficient understanding of fundamental correlations among different products still hinders the development of universal catalyst design strategies. Herein, we first discover that the surface *CO coverage is stable over a wide potential range and reveal a linear correlation between the partial current densities of CH4 and C2 products in this potential range, also supported by the theoretical kinetic analysis. Based on the mechanism that *CHO is the common intermediate in the formation of both CH4 (*CHO â†’ CH4) and C2 (*CHO + *CO â†’ C2), we then unravel that this linear correlation is universal and the slope can be varied by tuning the surface *H or *CO coverage to promote the selectivity of CH4 or C2 products, respectively. As proofs-of-concept, using carbon-coated Cu particles, the surface *H coverage can be increased to enhance CH4 production, presenting a high CO2-to-CH4 Faradaic efficiency ( [Formula: see text] ∼52%) and an outstanding CH4 partial current density of -337 mA cm-2. On the other hand, using an Ag-doped Cu catalyst, the CO2RR selectivity is switched to the C2 pathway, with a substantially promoted [Formula: see text] of 79% and a high partial current density of -421 mA cm-2. Our discovery of tuning intermediate coverages suggests a powerful catalyst design strategy for different CO2 electroreduction pathways.

4.
Small ; 16(40): e2004380, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32924278

RESUMO

Rhodium (Rh)-based catalysts may solve the long-standing inefficient oxidation of ethanol for direct ethanol fuel cells (DEFCs); however, the performance of ethanol oxidation reaction (EOR) on existing Rh-based catalysts are far limited. Herein, the Rh-Pb catalysts are synthesized by building Pb and Pb oxide around Rh nanodomain, which shows highly efficient splitting CC bond and facile further oxidation of as-generated C1 intermediates (COad and CHx fragments). It exhibits an ever-highest EOR peak mass activity of ≈2636 mA mg-1 Rh among Rh-based catalysts in alkaline media. Meanwhile, its anodic current remains ≈50% even after a 4 h durability test at 0.53 V versus RHE. As for the C1-pathway selectivity, in situ infrared adsorption spectral (IRAS) results demonstrate that it could significantly improve the production of CO2 . More directly, the apparent faraday efficiency of EOR C1 pathway is estimated to be as high as 20% (at 0.53 V versus RHE). This Rh-Pb catalyst could hold great promise for developing the commercial DEFCs.

5.
Angew Chem Int Ed Engl ; 59(47): 20826-20830, 2020 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-32767494

RESUMO

A methanol economy will be favored by the availability of low-cost catalysts able to selectively oxidize methanol to formate. This selective oxidation would allow extraction of the largest part of the fuel energy while concurrently producing a chemical with even higher commercial value than the fuel itself. Herein, we present a highly active methanol electrooxidation catalyst based on abundant elements and with an optimized structure to simultaneously maximize interaction with the electrolyte and mobility of charge carriers. In situ infrared spectroscopy combined with nuclear magnetic resonance spectroscopy showed that branched nickel carbide particles are the first catalyst determined to have nearly 100 % electrochemical conversion of methanol to formate without generating detectable CO2 as a byproduct. Electrochemical kinetics analysis revealed the optimized reaction conditions and the electrode delivered excellent activities. This work provides a straightforward and cost-efficient way for the conversion of organic small molecules and the first direct evidence of a selective formate reaction pathway.

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