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1.
Inorg Chem ; 63(4): 2131-2137, 2024 Jan 29.
Artículo en Inglés | MEDLINE | ID: mdl-38212991

RESUMEN

The electrochemical conversion of CO2 into controllable syngas (CO/H2) over a wide potential range is challenging. The main electrocatalysts are based on the noble metals Au (Ag) or heavy metal Pb. The development of alternative nonprecious catalysts is of paramount importance for practice. In this work, a simple coordination confined thermal pyrolysis method has been developed for the synthesis of Ni single-atom catalyst loaded onto nitrogen-doped commercial carbon. The catalyst is in the form of NiN3-C, which exhibits a high-performance electrocatalytic reduction of CO2 toward producing syngas with Faraday efficiencies of 62.28% of CO and 36.7% of H2. The Gibbs free energies of COOH* and H* on the NiN3-C structure were estimated by using density functional theory (DFT). The formation of COOH* intermediate is the speed-limiting step in the process, with ΔG COOH* being 0.7 eV, while H* is the speed-limiting step in the hydrogen evolution, respectively. This work provides a feasible method for the achievement of nonprecious catalysts for the resourceful use of CO2.

2.
Sci Total Environ ; 905: 167629, 2023 Dec 20.
Artículo en Inglés | MEDLINE | ID: mdl-37838042

RESUMEN

Integrated rice-crayfish farming is an ecological rice farming mode. However, limited research has examined the comprehensive impacts of greenhouse gas (GHG) emissions, nitrogen (N) uptake, and N utilization in rice under this farming modality. Herein, a dual-factor experiment was performed from 2021 to 2022 to assess the comprehensive impacts of N application and rice farming mode on greenhouse gas (GHG) emissions, N uptake, N utilization, and rice yield in paddy fields. Under N application, the rice-crayfish co-culture exhibits a 2.3 % decrease in global warming potential (GWP) and a 17.3 % increase in greenhouse gas intensity relative to the rice monoculture. Moreover, the N uptake of rice within the rice-crayfish co-culture is 5.2 %-10.4 % higher than that in the rice monoculture. However, owing to low rice yield under the rice-crayfish co-culture, its N partial factor productivity decreases by 5.6 %-22.6 %, while N agronomic efficiency is reduced by 18.3 %-46.9 % compared with the rice monoculture. In addition, N application significantly inhibits CH4 emissions from paddy fields in the rice-crayfish co-culture mode. Compared with no N application, the CH4 emissions and GWP of N-applied treatment are decreased by 12.1 %-31.0 % and 6.0 %-15.8 %, respectively. Hence, N regulation might reduce GHG emissions in rice-aquatic animal co-culturing agriculture. Collectively, the results of this study suggest that switching from a rice monoculture to rice-crayfish co-culture can mitigate GHG emissions and promote rice N uptake; however, continuously improving the productivity of co-culturing agriculture is key to achieving high N utilization efficiency and low environmental impact.


Asunto(s)
Gases de Efecto Invernadero , Oryza , Animales , Gases de Efecto Invernadero/análisis , Astacoidea , Nitrógeno , Suelo , Metano/análisis , Óxido Nitroso/análisis , Agricultura/métodos , Fertilizantes/análisis
3.
J Sci Food Agric ; 103(2): 968-975, 2023 Jan 30.
Artículo en Inglés | MEDLINE | ID: mdl-36260409

RESUMEN

BACKGROUND: Rice-duck coculture is an ecological agricultural mode; however, the nutritional and environmental benefits of transforming from conventional rice monoculture to rice-duck coculture are unknown. Based on survey data and the life-cycle assessment approach, this study conducted a carbon footprint evaluation of conventional rice monoculture (CR), organic rice monoculture (OR), and organic rice-duck coculture (ORD) using different functional units. RESULTS: The carbon footprint per hectare of ORD (7842 ± 284 kg CO2 eq ha-1 ) was slightly lower than that of CR (7905 ± 412 kg CO2 eq ha-1 ), while higher than that of OR (7786 ± 235 kg CO2 eq ha-1 ). Although the rice yield of ORD was slightly lower than that of CR, its nutrient density unit (NDU) did not decrease significantly due to the additional duck yield. Thus, the carbon footprint per NDU of ORD was significantly lower than that of OR by 24.3% (P < 0.05) and was 5.8% higher than that of CR, but this was not statistically significant. Due to the higher economic profits of ORD, its unit of carbon footprint per economic profit was significantly reduced (by 47.1-75.7%) compared with the other two farming modes, while the net ecosystem economic budget was significantly increased by 98.5-341.9% (P < 0.05). CONCLUSION: Transforming from a rice monoculture to a coculture system will contribute to a win-win situation for human health and environmental sustainability. This study highlighted the abundant nutritional output function of the rice-duck coculture and analyzed the urgency and necessity of transitioning from traditional agriculture to ecological agriculture from the production and consumption perspectives. © 2022 Society of Chemical Industry.


Asunto(s)
Patos , Oryza , Animales , Humanos , Ecosistema , Dióxido de Carbono , Técnicas de Cocultivo , Huella de Carbono , Agricultura , China
4.
Foods ; 11(23)2022 Nov 27.
Artículo en Inglés | MEDLINE | ID: mdl-36496637

RESUMEN

Previous studies have mainly focused on cadmium (Cd) contamination in conventional rice monocultures, and no research on rice-crayfish coculture has been reported. In this study, a Cd-contaminated (0−30 mg kg−1) rice-crayfish co-culture system was established by adding exogenous Cd. The results showed that the Cd concentration in each tissue of rice and each organ of crayfish increased with increasing soil Cd concentration. Specifically, the Cd concentration in each rice tissue was as follows: root > stem > leaf ≈ panicle > grain > brown rice, and the jointing and heading stages were critical periods for the rapid enrichment of Cd in the aboveground tissues of rice. The Cd concentration in each organ of crayfish was as follows: hepatopancreas > gut > gill ≈ exoskeleton > abdominal muscle. Cd was gradually enriched in the abdominal muscle after 30 days of coculture between crayfish and rice. Pearson's correlation analysis showed that the soil's total Cd concentration, available Cd concentration, and water Cd concentration were positively correlated with Cd content in various tissues of rice and various organs of crayfish, whereas EC and TDS in water were markedly related to rice stems, leaves, stalks, and small crayfish. According to the maximum limit of Cd in grain (0.2 mg kg−1) and crustacean aquatic products (0.5 mg kg−1) in China, the safe threshold of soil Cd for rice and crayfish under the rice-crayfish coculture system is 3.67 and 14.62 mg kg−1, respectively. Therefore, when the soil Cd concentration in the rice-crayfish coculture system exceeds 3.67 mg kg−1, the safety risk to humans through the consumption of food from this coculture system will increase. This study provides a theoretical basis for safe food production in a rice-crayfish coculture system using the established Cd pollution model.

5.
Small ; 18(14): e2105226, 2022 04.
Artículo en Inglés | MEDLINE | ID: mdl-35182021

RESUMEN

Tailoring the structure of metal components and interaction with their anchored substrates is essential for improving the catalytic performance of supported metal catalysts; the ideal catalytic configuration, especially down to the range of atomic layers, clusters, and even single atoms, remains a subject under intensive study. Here, an Ir-on-MXene (Mo2 TiC2 Tx ) catalyst with controlled morphology changing from nanoparticles down to flattened atomic layers, and finally ultrathin layers and single atoms dispersed on MXene nanosheets at elevated temperature, is presented. The intermediate structure, consisting of mostly Ir atomic layers, shows the highest activity toward the hydrogen evolution reaction (HER) under industry-compatible alkaline conditions. In addition, the better HER activity of Ir atomic layers than that of single atoms suggests that the former serves as the main active sites. Detailed mechanism analysis reveals that the nanoparticle re-dispersion process and Ir atomic layers with a moderate interaction to the substrate associate with unconventional electron transfer from MXene to Ir, leading to suitable H* adsorption. The results indicate that the structural design is important for the development of highly efficient catalysts.


Asunto(s)
Iridio , Nanopartículas , Adsorción , Catálisis , Hidrógeno
6.
ACS Appl Mater Interfaces ; 14(1): 1452-1459, 2022 Jan 12.
Artículo en Inglés | MEDLINE | ID: mdl-34958544

RESUMEN

Generating hydrogen by water electrolysis is a promising and sustainable approach to the production of a green energy carrier, but the sluggish kinetics of the oxygen evolution reaction (OER) at anode leads to a high working potential. Replacing OER with electro-oxidation of organics driven at a low potential offers an effective way to accelerate the sluggish anode reaction, and thus increase hydrogen evolution in water-splitting. Herein, we have prepared a Ru nanoparticles on N-doped carbon nanotubes (Ru-NPs@NCNTs) to implement electro-oxidation of benzyl alcohol toward reducing the anodic potential in watersplitting. The potential of the anode reaction is remarkably decreased from 1.76 to 1.19 V vs RHE at a current density of 10 mA cm-2 with the assistance of a Ru-NPs catalyst. Furthermore, 100% selectivity and 95% yield of valuable benzaldehyde were achieved simultaneously. The Ru-NPs also exhibits good durability and wide applicability to other alcohols. The high performance of Ru-NPs is mainly attributed to the unique horizontal adsorption configuration of benzyl alcohol with surface atoms of the catalyst, shortening the distance between the •OH group and Ru atoms, and increasing the activation rate of the •OH group. This work presents a feasible strategy to boost water-splitting performance and concurrently produce value-added organics under mild conditions.

7.
ACS Nano ; 15(5): 7946-7974, 2021 May 25.
Artículo en Inglés | MEDLINE | ID: mdl-33988980

RESUMEN

Carbon nanotube functional materials (CNTFMs) represent an important research field in transforming nanoscience and nanotechnology into practical applications, with potential impact in a wide realm of science, technology, and engineering. In this review, we combine the state-of-the-art research activities of CNTFMs with the application prospect, to highlight critical issues and identify future challenges. We focus on macroscopic long fibers, thin films, and bulk sponges which are typical CNTFMs in different dimensions with distinct characteristics, and also cover a variety of derived composite/hierarchical materials. Critical issues related to their structures, properties, and applications as robust conductive skeletons or high-performance flexible electrodes in mechanical and electronic devices, advanced energy conversion and storage systems, and environmental areas have been discussed specifically. Finally, possible solutions and directions are proposed for overcoming current obstacles and promoting future efforts in the field.

8.
ACS Nano ; 13(4): 3982-3991, 2019 Apr 23.
Artículo en Inglés | MEDLINE | ID: mdl-30892017

RESUMEN

Lithium-sulfur (Li-S) batteries are next-generation energy storage systems with high energy density, and the rate performance is a very important consideration for practical applications. Recent approaches such as introducing catalytic materials to facilitate polysulfide conversion have been explored, yet the results remain unsatisfactory. Here, we present an optimized Li-S electrode featured by a large amount of highly dispersed Co3S4 nanoparticles (∼10 nm in size) throughout a hierarchical carbon nanostructure hybridized from ZIF-67 and carbon nanotube (CNT) sponge. This enables homogeneous distribution and close contact between infiltrated sulfur and Co3S4 nanoparticles within the ZIF-67-derived N-doped carbon nanocubes, leading to effective chemical interaction with polysulfides, maximum catalytic effect and enhanced lithium ion diffusion, while the built-in three-dimensional CNT network ensures high electrical conductivity of the electrode. As a consequence, the Li-S battery exhibits both extraordinary rate performance by maintaining a capacity of ∼850 mAh g-1 at very high charge/discharge rate (5 C) and long-term cycling stability with 85% retention after 1000 cycles at 5 C (an average capacity fading rate of only 0.0137% per cycle).

9.
Chem Commun (Camb) ; 52(28): 5023-6, 2016 Apr 11.
Artículo en Inglés | MEDLINE | ID: mdl-26984304

RESUMEN

〈100〉-oriented Pt and Pt-Rh supercrystals were directly synthesized in N,N-dimethylformamide (DMF) solution. DMF was demonstrated to serve as the facet-specific agent of the (100) facets and the driving force for the self-assembly of Pt and Pt-Rh building blocks due to the strong bonding interaction between metal atoms on the (100) facets and the carbonyl group of DMF.


Asunto(s)
Dimetilformamida/química , Compuestos Organometálicos/síntesis química , Platino (Metal)/química , Rodio/química , Adsorción , Cristalización , Compuestos Organometálicos/química , Tamaño de la Partícula , Propiedades de Superficie
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