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1.
Bioresour Technol ; 412: 131406, 2024 Aug 31.
Artículo en Inglés | MEDLINE | ID: mdl-39222863

RESUMEN

Microalgae as a promising approach for wastewater treatment, has challenges in directly treating digested piggery wastewater (DPW) with high ammonia nitrogen (NH4+-N) concentration. To improve the performance of microalgae in DPW treatment, straw was employed as a substrate to form a straw-microalgae biofilm. The results demonstrated that the straw-microalgae biofilm achieved the highest NH4+-N removal rate of 193.2 mg L-1 d-1, which was 28.8 % higher than that of culture system without straw. The final NH4+-N concentration in the effluent met the discharge standard of 5 mg L-1. Furthermore, the total organic carbon (TOC) released from straw facilitated bacterial proliferation and the secretion of extracellular polymeric substances (EPS). The EPS and TOC increased the suspension viscosity and surface tension, thereby enhancing the residence time of CO2 in the liquid phase and promoting CO2 fixation. This study presented a novel method for the biological treatment of high-ammonia-nitrogen DPW.

2.
Anal Chem ; 2024 Sep 04.
Artículo en Inglés | MEDLINE | ID: mdl-39233361

RESUMEN

The enzymatic depolymerization is a promising route to valorize the lignin polymers by turning the cross-linked polymers into monomers or oligomers. However, the lignin polymers cannot be effectively converted into small chemicals, as the oligomers are prone to polymerization, which is particularly challenging to monitor and thus regulate. Here, we develop a microstructured fiber Bragg grating (mFBG) sensor to probe the dynamic polymerization process of typical lignin oligomer surrogates─guaiacol (monomer) and guaiacylglycerol-ß-guaiacyl ether (GBG, dimer)─catalyzed by laccase in an operando way. The mFBG sensor was developed with its reliability well validated by control experiments at first. Further, operando monitoring of the polymerization reaction process of the typical lignin monomer (i.e., guaiacol) and dimer (guaiacylglycerol-ß-guaiacyl ether, GBG) was demonstrated under various conditions with the mFBG sensor. The GC-MS and UV-vis absorption measurements were carried out as a further check. Finally, the specific polymerization characteristics and reaction mechanism were studied. The mFBG sensor enables operando monitoring of the heterogeneous polymerization process of lignin monomers and oligomers and can potentially be tailored to probe more complex lignin depolymerization processes and unveil enzymatic synergistic mechanisms for the biological transition of biomass.

3.
J Phys Chem Lett ; 15(34): 8877-8895, 2024 Aug 29.
Artículo en Inglés | MEDLINE | ID: mdl-39171577

RESUMEN

Optofluidics, which utilizes the interactions between light and fluids to realize various functions, has garnered increasing attention owing to the advantages of operational simplicity, exceptional flexibility, rapid response, etc. As one of the typical light-fluid interactions, the localized photothermal effect serving as a stimulus has been widely used for fluid manipulation. Particularly, significant progress on photothermal-driven droplet manipulation has been made. In this perspective, recent advancements in localized photothermal effect driven droplet manipulation are summarized. First, the photothermal manipulation of droplets on open surfaces is outlined. An attractive droplet manipulation of light droplet levitation above the gas-liquid interface via localized photothermal effect is then discussed. Besides, the photothermal-driven manipulation of droplets in an immiscible liquid phase is also discussed. Although promising, further development of photothermal-driven droplet manipulation is still needed. The challenges and perspectives of this light droplet manipulation strategy for broad implementation are summarized, which will help future studies and applications.

4.
J Phys Chem Lett ; 15(32): 8367-8377, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39115282

RESUMEN

The rational design of photocatalysts for improving the conversion of solar energy into hydrogen is a promising route for achieving carbon neutrality. Herein, we couple plasmonic titanium nitride (TiN) with highly crystalline potassium-doped polymeric carbon nitride (PPCN) to construct a PPCN/TiN ohmic junction. Such an ohmic junction not only broadens the absorption spectrum but also inhibits the recombination of electrons and holes. In addition, Pt nanoparticles are introduced into this ohmic junction to form plasmonic Pt-PPCN/TiN, improving the capture of hot electrons generated by TiN and thereby promoting the dissociation of the O-H bond in H2O. The energy barrier decreases from 0.7 to 0.2 eV. Enhanced separation of carrier, activation of water molecules, and capture of hot electrons are jointly promoting photo-thermo catalytic hydrogen production. Therefore, under full-spectrum irradiation, the hydrogen production rate of Pt-PPCN/TiN reaches 19 085 µmol g-1 h-1. This novel plasmonic photocatalyst is promising for full-spectrum photo-thermo catalytic hydrogen production.

5.
J Phys Chem Lett ; 15(26): 6736-6742, 2024 Jul 04.
Artículo en Inglés | MEDLINE | ID: mdl-38905537

RESUMEN

Developing high-performance electrodes for the all-aqueous thermally regenerative ammonia battery (ATRB) system, serving as superior substitutes for commercial carbon cloth electrodes, is anticipated to enhance performance, yet it lacks effective guidance and research. In this work, theoretical analysis is initially used to evaluate the effective conversion and adsorption capacity of nitrogen and sulfur co-doped carbon with respect to copper ion by density functional theory calculation. On the basis of this concept, the nitrogen and sulfur co-doped biomass-derived porous carbon electrode (DGC) is prepared using natural porous carbon materials and thiourea. Compared with commercial carbon cloth electrodes, ATRB with DGC achieves a significant improvement in maximum power density of 49.2%. Via optimization of the doping conditions, the active sites can be effectively regulated to boost charge transfer at the reaction interface. Furthermore, the rapid charge transfer can match the excellent mass transfer performance, generating an impressive net power density of 847.5 W/m2.

6.
ACS Appl Mater Interfaces ; 16(26): 33336-33346, 2024 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-38907693

RESUMEN

Developing earth-abundant transition metal electrodes with high activity and durability is crucial for efficient and cost-effective hydrogen production. However, numerous studies in the hydrogen evolution reaction (HER) primarily focus on improving the inherent activity of catalysts, and the critical influence of gas-liquid countercurrent transport behavior is often overlooked. In this study, we introduce the concept of separate-path gas-liquid transport to alleviate mass transport losses for the HER by developing a novel hierarchical porous Ni-doped cobalt phosphide electrode (CoNix-P@Ni). The CoNix-P@Ni electrodes with abundant microvalleys and crack structures facilitate the gas-liquid cotransport by separating the bubble release and water supply paths. Visualization and numerical simulation results demonstrate that cracks primarily serve as water supply paths, with capillary pressure facilitating the transport of water from the cracks to the microvalleys. This process ensures the continuous wetting of electrolytes in the electrode, reduces hydrogen supersaturation near the active site, and increases hydrogen transport flux to the microvalleys for accelerating bubble growth. Additionally, the microvalleys act as preferential sites for bubble evolution, preventing bubble coverage on other active sites. By regulating the amount of nickel, the CoNi1-P@Ni electrode exhibited the smallest and densest microvalleys and cracks, achieving superior HER performance with an overpotential of 51 mV at 10 mA cm-2. The results offer a promising direction for constructing high-performance HER electrodes.

7.
Phys Chem Chem Phys ; 26(23): 16514-16520, 2024 Jun 12.
Artículo en Inglés | MEDLINE | ID: mdl-38832437

RESUMEN

The interfacial correlation factor f(m,x), where m refers to the interaction among ice, water and the substrate and x refers to the ratio of the critical nucleation size to the surface topography characteristic size of the substrate, plays a crucial role in the classical theory of heterogeneous ice nucleation as it significantly impacts the energy of nucleation. Generally, a smaller value of f(m,x) indicates a higher propensity for ice nucleation. The degree of structural compatibility between ice and the substrate greatly influences f(m,x), particularly on specific substrates. Several approaches have been proposed to calculate the lattice matching based on this idea, which allows whether a surface is favorable for nucleation to be determined. However, none of these methods adequately correlates the mismatch index with ice growth phenomena. In this paper, we embarked on a new attempt to calculate the mismatch index by combining the lattice parameter and Miller index (LPMI). Droplet freezing experiments have been carried out on α-Al2O3 and silicon surfaces with different Miller indices to verify the rationality of the LPMI method. Furthermore, we validated the LPMI method extensively against other works and further demonstrated its readiness, accuracy and universality for freezing problems. The results consistently show that δd = 2|di - ds|/(di + ds) with interplanar spacing more accurately predicts heterogeneous ice nucleation rates across a wide range of substrates than δ1 = (ai - as)/ai with the lattice parameter of ice and the substrate and is more generally applicable than δ2D = (di - di)/di with the distances between two adjacent and congener atoms on the same plane. We believe that the proposed approach will aid in the selection of substrates for promoting or inhibiting heterogeneous nucleation on a specific substrate.

8.
Environ Res ; 256: 119245, 2024 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-38810821

RESUMEN

Microalgae have been renowned as the most promising energy organism with significant potential in carbon fixation. In the large-scale cultivation of microalgae, the 3D porous substrate with higher specific surface area is favorable to microalgae adsorption and biofilm formation, whereas difficult for biofilm detachment and microalgae harvesting. To solve this contradiction, N-isopropylacrylamide, a temperature-responsive gels material, was grafted onto the inner surface of the 3D porous substrate to form temperature-controllable interface wettability. The interfacial free energy between microalgae biofilm and the substrates increased from -63.02 mJ/m2 to -31.89 mJ/m2 when temperature was lowered from 32 °C to 17 °C, weakening the adsorption capacity of cells to the surface, and making the biofilm detachment ratio increased to 50.8%. When further cooling the environmental temperature to 4 °C, the detachment capability of microalgae biofilm kept growing. 91.6% of the cells in the biofilm were harvesting from the 3D porous substrate. And the biofilm detached rate was up to 19.84 g/m2/h, realizing the temperature-controlled microalgae biofilm harvesting. But, microalgae growth results in the secretion of extracellular polymeric substances (EPS), which enhanced biofilm adhesion and made cell detachment more difficult. Thus, ultrasonic vibration was used to reinforce biofilm detachment. With the help of ultrasonic vibration, microalgae biofilm detached rate increased by 143.45% to 41.07 g/m2/h. These findings provide a solid foundation for further development of microalgae biofilm detachment and harvesting technology.


Asunto(s)
Biopelículas , Geles , Microalgas , Temperatura , Biopelículas/crecimiento & desarrollo , Microalgas/crecimiento & desarrollo , Porosidad , Geles/química , Acrilamidas/química
9.
BMC Infect Dis ; 24(1): 457, 2024 Apr 30.
Artículo en Inglés | MEDLINE | ID: mdl-38689228

RESUMEN

BACKGROUND: HIV-tuberculosis (HIV-TB) co-infection is a significant public health concern worldwide. TB delay, consisting of patient delay, diagnostic delay, treatment delay, increases the risk of adverse anti-TB treatment (ATT) outcomes. Except for individual level variables, differences in regional levels have been shown to impact the ATT outcomes. However, few studies appropriately considered possible individual and regional level confounding variables. In this study, we aimed to assess the association of TB delay on treatment outcomes in HIV-TB co-infected patients in Liangshan Yi Autonomous Prefecture (Liangshan Prefecture) of China, using a causal inference framework while taking into account individual and regional level factors. METHODS: We conducted a study to analyze data from 2068 patients with HIV-TB co-infection in Liangshan Prefecture from 2019 to 2022. To address potential confounding bias, we used a causal directed acyclic graph (DAG) to select appropriate confounding variables. Further, we controlled for these confounders through multilevel propensity score and inverse probability weighting (IPW). RESULTS: The successful rate of ATT for patients with HIV-TB co-infection in Liangshan Prefecture was 91.2%. Total delay (OR = 1.411, 95% CI: 1.015, 1.962), diagnostic delay (OR = 1.778, 95% CI: 1.261, 2.508), treatment delay (OR = 1.749, 95% CI: 1.146, 2.668) and health system delay (OR = 1.480 95% CI: (1.035, 2.118) were identified as risk factors for successful ATT outcome. Sensitivity analysis demonstrated the robustness of these findings. CONCLUSIONS: HIV-TB co-infection prevention and control policy in Liangshan Prefecture should prioritize early treatment for diagnosed HIV-TB co-infected patients. It is urgent to improve the health system in Liangshan Prefecture to reduce delays in diagnosis and treatment.


Asunto(s)
Coinfección , Infecciones por VIH , Puntaje de Propensión , Tuberculosis , Humanos , Infecciones por VIH/complicaciones , Infecciones por VIH/tratamiento farmacológico , Femenino , Masculino , Coinfección/tratamiento farmacológico , Coinfección/epidemiología , Adulto , China/epidemiología , Tuberculosis/tratamiento farmacológico , Tuberculosis/complicaciones , Persona de Mediana Edad , Resultado del Tratamiento , Antituberculosos/uso terapéutico , Tiempo de Tratamiento/estadística & datos numéricos , Diagnóstico Tardío
10.
Plant Foods Hum Nutr ; 79(2): 367-373, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38489084

RESUMEN

The immunostimulatory effects and the involved molecular mechanisms of polysaccharides from hawthorn fruit (Crataegus spp.) have not been well understood. In this study, the chemical composition, monosaccharide composition, uronic acid content, and structural features of hawthorn fruit polysaccharides (HFP) and the two collected fractions were analyzed. Both AF1-2 and AF2 have pectic-like structural features rich in galacturonic acid. AF2 showed superior proinflammatory effects on macrophages which significantly increased the secretion of pro-inflammatory cytokines interleukin-1ß, interleukin-6, and tumor necrosis factor-α, but not AF1-2. AF2 was found to activate the nuclear factor-κB signaling pathway with suppressed expression of IκBα but up-regulated expression of p-IκBα and nuclear factor-κB P65. The surface binding site of AF2 on macrophage cells was characterized and toll like receptor-4 was responsible for AF2 induced activation of down-stream nuclear factor-κB signaling pathways. AF2 from hawthorn fruit could be potentially used as a natural source of immunomodulator in functional foods.


Asunto(s)
Crataegus , Frutas , Factores Inmunológicos , Macrófagos , FN-kappa B , Polisacáridos , Transducción de Señal , Receptor Toll-Like 4 , Crataegus/química , Receptor Toll-Like 4/metabolismo , Polisacáridos/farmacología , Transducción de Señal/efectos de los fármacos , Macrófagos/efectos de los fármacos , Macrófagos/metabolismo , Frutas/química , FN-kappa B/metabolismo , Ratones , Animales , Factores Inmunológicos/farmacología , Células RAW 264.7 , Extractos Vegetales/farmacología , Extractos Vegetales/química , Factor de Necrosis Tumoral alfa/metabolismo , Citocinas/metabolismo , Interleucina-6/metabolismo , Interleucina-1beta/metabolismo , Ácidos Hexurónicos
11.
Environ Monit Assess ; 196(4): 360, 2024 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-38472494

RESUMEN

As a crucial ecological protection area in China, the Southern hilly red soil region is characterized by uneven spatial and temporal distribution of ecological landscape elements, unpredictable and changeable interrelationships between them, diversified driving factors, and lack of comprehensive consideration of ecosystem services. In order to better understand the interaction between ecosystem services, restore regional ecology, and promote sustainable development, the evolution law and influencing mechanism of ecosystem services and their driving factors are quantitatively analyzed in the study. Based on simulations of different ecosystem services from 2000 to 2020, their spatial and temporal changes and the contributions of main drivers are quantified, their trade-offs and synergies are analyzed, and the changing rules under the influence of natural factors and socioeconomic factors are explored. The results show that (1) the crop production significantly increases in the southwest and north regions, the habitat quality decreases in urban and coastal areas, and the soil retention and water yield show an increasing trend from west to east. (2) Land use/cover is the main driver of carbon storage and habitat quality variation, and precipitation is an important driver of water yield spatial variation. (3) The crop production and the other four ecosystem services show a trade-offs relationship, and the relationship between supporting services and regulating services is the synergetic. (4) The altitude weakens the synergistic relationship between soil retention and habitat quality/carbon storage, while it enhances the synergistic relationship between soil retention and water yield. Driven by precipitation factors, ecosystem services related to water yield have significant differences in the change. The population density enhances the trade-offs of crop production and soil retention, as well as the synergistic relationship between soil retention and habitat quality/carbon storage. In different land use/cover (LULC), the influence of urban land on ecosystem services relationship change is more obvious. Overall, this study can provide scientific bases and policy suggestions for ecosystem protection/restoration in the red soil region of Southern China, which has an important theoretical and practical significance.


Asunto(s)
Ecosistema , Suelo , Conservación de los Recursos Naturales/métodos , Monitoreo del Ambiente/métodos , China , Carbono , Agua
12.
Neural Regen Res ; 19(10): 2157-2174, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38488550

RESUMEN

Traumatic brain injury is a serious medical condition that can be attributed to falls, motor vehicle accidents, sports injuries and acts of violence, causing a series of neural injuries and neuropsychiatric symptoms. However, limited accessibility to the injury sites, complicated histological and anatomical structure, intricate cellular and extracellular milieu, lack of regenerative capacity in the native cells, vast variety of damage routes, and the insufficient time available for treatment have restricted the widespread application of several therapeutic methods in cases of central nervous system injury. Tissue engineering and regenerative medicine have emerged as innovative approaches in the field of nerve regeneration. By combining biomaterials, stem cells, and growth factors, these approaches have provided a platform for developing effective treatments for neural injuries, which can offer the potential to restore neural function, improve patient outcomes, and reduce the need for drugs and invasive surgical procedures. Biomaterials have shown advantages in promoting neural development, inhibiting glial scar formation, and providing a suitable biomimetic neural microenvironment, which makes their application promising in the field of neural regeneration. For instance, bioactive scaffolds loaded with stem cells can provide a biocompatible and biodegradable milieu. Furthermore, stem cells-derived exosomes combine the advantages of stem cells, avoid the risk of immune rejection, cooperate with biomaterials to enhance their biological functions, and exert stable functions, thereby inducing angiogenesis and neural regeneration in patients with traumatic brain injury and promoting the recovery of brain function. Unfortunately, biomaterials have shown positive effects in the laboratory, but when similar materials are used in clinical studies of human central nervous system regeneration, their efficacy is unsatisfactory. Here, we review the characteristics and properties of various bioactive materials, followed by the introduction of applications based on biochemistry and cell molecules, and discuss the emerging role of biomaterials in promoting neural regeneration. Further, we summarize the adaptive biomaterials infused with exosomes produced from stem cells and stem cells themselves for the treatment of traumatic brain injury. Finally, we present the main limitations of biomaterials for the treatment of traumatic brain injury and offer insights into their future potential.

13.
Adv Mater ; 36(15): e2305711, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38342600

RESUMEN

High-performance proton exchange membrane (PEM) is crucial for the proton exchange membrane fuel cell (PEMFC). Herein, a novel "self-enhanced" PEM is fabricated for the first time, which is composed of perfluorinated sulfonic acid (PFSA) resin and its own nanofibers as reinforcement. With this strategy, the interfacial compatibility issue of conventional fiber-reinforced membranes is fully addressed and up to 80 wt% loading of PFSA nanofibers can be incorporated. Furthermore, on account of chain orientation within the PFSA nanofiber, single fiber exhibits super-high conductivity of 1.45 S cm-1, leading to state-of-the-art proton conductivity (1.1 S cm-1) of the as-prepared "self-enhanced" PEM so far, which is an order of magnitude increase compared with the bulk PFSA membrane (0.29 S cm-1). It surpasses any commercial PEM including the popular GORE-SELECT and Nafion HP membranes and is the only PEM with conductivity at 100 S cm-1 level. In addition, the mechanical strength and swelling ratio of membranes are both substantially improved simultaneously. Based on the high-performance "self-enhanced" PEM, high peak power densities of up to 3.6 W cm-2 and 1.7 W cm-2 are achieved in H2-O2 and H2-Air fuel cells, respectively. This strategy can be applied in any polymeric electrolyte membrane.

14.
Small ; 20(25): e2309648, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38234134

RESUMEN

The utility of electrochemical active biofilm in bioelectrochemical systems has received considerable attention for harvesting energy and chemical products. However, the slow electron transfer between biofilms and electrodes hinders the enhancement of performance and still remains challenging. Here, using Fe3O4 /L-Cys nanoparticles as precursors to induce biomineralization, a facile strategy for the construction of an effective electron transfer pathway through biofilm and biological/inorganic interface is proposed, and the underlying mechanisms are elucidated. Taking advantage of an on-chip interdigitated microelectrode array (IDA), the conductive current of biofilm that is related to the electron transfer process within biofilm is characterized, and a 2.10-fold increase in current output is detected. The modification of Fe3O4/L-Cys on the electrode surface facilitates the electron transfer between the biofilm and the electrode, as the bio/inorganic interface electron transfer resistance is only 16% compared to the control. The in-situ biosynthetic Fe-containing nanoparticles (e.g., FeS) enhance the transmembrane EET and the EET within biofilm, and the peak conductivity increases 3.4-fold compared to the control. The in-situ biosynthesis method upregulates the genes involved in energy metabolism and electron transfer from the transcriptome analysis. This study enriches the insights of biosynthetic nanoparticles on electron transfer process, holding promise in bioenergy conversion.


Asunto(s)
Biopelículas , Transporte de Electrón , Técnicas Electroquímicas/métodos , Compuestos Ferrosos/química , Electrodos , Nanopartículas/química , Fuentes de Energía Bioeléctrica
15.
Adv Mater ; 36(1): e2305854, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37671789

RESUMEN

As a reliable energy-supply platform for wearable electronics, biosupercapacitors combine the characteristics of biofuel cells and supercapacitors to harvest and store the energy from human's sweat. However, the bulky preparation process and deep embedding of enzyme active sites in bioelectrodes usually limit the energy-harvesting process, retarding the practical power-supply sceneries especially during the complicated in vivo motion. Herein, a MXene/single-walled carbon nanotube/lactate oxidase hierarchical structure as the dual-functional bioanode is designed, which can not only provide a superior 3D catalytic microenvironment for enzyme accommodation to harvest energy from sweat, but also offers sufficient capacitance to store energy via the electrical double-layer capacitor. A wearable biosupercapacitor is fabricated in the "island-bridge" structure with a composite bioanode, active carbon/Pt cathode, polyacrylamide hydrogel substrate, and liquid metal conductor. The device exhibits an open-circuit voltage of 0.48 V and the high power density of 220.9 µW cm-2 at 0.5 mA cm-2 . The compact conformal adhesion with skin is successfully maintained under stretching/bending conditions. After repeatedly stretching the devices, there is no significant power attenuation in pulsed output. The unique bioelectrode structure and attractive energy harvesting/storing properties demonstrate the promising potential of this biosupercapacitor as a micro self-powered platform of wearable electronics.


Asunto(s)
Fuentes de Energía Bioeléctrica , Dispositivos Electrónicos Vestibles , Humanos , Electrónica , Catálisis
16.
Bioelectrochemistry ; 156: 108622, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38070364

RESUMEN

Microbial fuel cells (MFCs) are an emerging technology in renewable energy and waste treatment and the scale-up is crucial for practical applications. Undoubtedly, the analysis and comprehension of MFC operation necessitate essential information regarding the response of the current distribution to variable operating conditions, which stands as one of its significant dynamic characteristics. In this study, the dynamic responses of current distribution to external stimuli (external load, temperature, pH, and electrolyte concentration) were investigated by employing a segmented anode current collector in a liter-scale MFC. The results demonstrated that, with respect to the anodic segment close to the cathode, a major response of the segment current to changes in load, temperature and pH was observed while minor response to changes in ion concentration. It was also found that external stimuli-induced high current usually led to a worse current distribution while increasing electrolyte ion concentration could simultaneously improve the maximal power generation and current distribution. In addition, the response time of segment current to input stimulus followed the pattern of temperature ˃ pH ˃ ion concentration ˃ external load. The results and implication of this study would be helpful in enhancing the operational stability of scale-up MFCs in future practical application.


Asunto(s)
Fuentes de Energía Bioeléctrica , Temperatura , Electrodos , Electrólitos
17.
ACS Appl Mater Interfaces ; 15(46): 53429-53435, 2023 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-37957114

RESUMEN

In alkaline and neutral zero-gap CO2 electrolyzers, the carbon utilization efficiency of the electrocatalytic CO2 reduction to CO is less than 50% because of inherently homogeneous reactions. Utilization of the bipolar membrane (BPM) electrolyzer can effectively suppress (bi)carbonate formation and parasitic CO2 losses; however, an excessive concentration of H+ in the catalyst layer (CL) significantly hinders the activity and selectivity for CO2 reduction. Here, we report a microenvironment regulation strategy that controls the CL thickness and ionomer content to regulate local CO2 transport and the local pH within the CL. We report 80% faradaic efficiency of CO at a current density of 400 mA/cm2 without the use of a buffering layer, exceeding that of state-of-the-art catalysts with a buffering layer. A carbon utilization efficiency of 63.6% at 400 mA/cm2 is also obtained. This study demonstrates the significance of regulating the microenvironment of the CL in a BPM system.

18.
Langmuir ; 39(45): 16182-16190, 2023 Nov 14.
Artículo en Inglés | MEDLINE | ID: mdl-37906836

RESUMEN

Photoelectrochemical reduction of carbon dioxide (CO2) is a promising avenue to realize resourceful utilization of carbon dioxide and mitigate the energy shortage. Herein, a photocatalytic fuel cell with a bubbling fluidized cathode (PFC-BFC) is proposed to increase the performance of the photocatalytic CO2 reduction reaction (CO2RR). Titanium carbide (Ti3C2) is first used as a fluidized cathode catalyst with the dual features of superior capacitance and high CO2RR catalytic activity. Compared with the conventional PFC system, the as-proposed PFC-BFC system exhibits a higher gas production performance. Particularly, the generation rate and Faraday efficiency for CH4 production reach to 37.2 µmol g-1 h-1 and 72%, which are 10.9 and 6.5 times higher than that of the conventional PFC system, respectively. The bubbling fluidized cathode allows a rapid electron transfer between catalysts and the current collector and an efficient diffusion of catalysts in the whole solution, thus remarkably increasing the effective reaction area of the CO2RR. In addition, the fluidized reaction mechanism of charging/discharging-coupled CO2RR is investigated. Significantly, a magnified PFC-BFC system is designed and exhibits a similar gas generation rate compared to that of the small-scale system, indicating a good potential of scaling up in the industry applications. These results demonstrated that the proposed PFC-BFC system can maximize the utilization of catalyst active sites and enhance the reaction kinetics, providing an alternative design for the application of CO2RR.

19.
Soft Matter ; 19(38): 7323-7333, 2023 Oct 04.
Artículo en Inglés | MEDLINE | ID: mdl-37727081

RESUMEN

Flexible control of droplet transportation is crucial in various applications but is constrained by liquid-solid friction. The development of biomimetic lubricant-impregnated slippery surfaces provides a new solution for flexible manipulation of droplet transportation. Herein, a light strategy is reported for flexibly controlling droplet transportation on photosensitive lubricant-impregnated slippery surfaces. Owing to the localized heating effect of a focused laser beam via photothermal conversion, the resultant thermal Marangoni flow and horizontal component of the surface tension associated with the asymmetric wetting ridges are together responsible for actuating droplet transportation. It is found that the asymmetry of the wetting ridge is dominated by the thickness of the infused oil layer, which directly affects the droplet transportation. The feasibility of this light strategy is also demonstrated by uphill movement, droplet coalescence, and chemical reaction. This study provides a new design for potential applications in open droplet microfluidics, analytical chemistry, diagnosis, etc.

20.
Lab Chip ; 23(19): 4287-4301, 2023 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-37682034

RESUMEN

Flexible and precise manipulation of droplet transport is of significance for scientific and engineering applications, but real-time and on-demand droplet manipulation remains a challenge. Herein, we report a strategy using light for the outstanding manipulation of binary droplet motion on a high-energy surface and reveal the underlying mechanism. Upon irradiation to a substrate by a focused light beam, the substrate can provide a localized heating source via photothermal conversion, and a binary droplet can be flexibly transported on a high-energy surface with free contact-line pinning, exhibiting light-propelled droplet transport. We theoretically showed that the surface tension gradient across the droplet interface resulting from the localized photothermal effect is responsible for actuating droplet transport. Remarkably, the high reconfigurability and flexibility of light allowed for binary droplet transport with dynamically tunable velocity and direction as well as arbitrary trajectory assisted by 2D channels on a high-energy surface. Complex droplet transportation, controllable droplet coalescence, and anti-gravity motion were realized. The promising applicability of this light-fueled droplet platform was also demonstrated by directional transport of biosample droplets containing DNA molecules and cells, as well as successional microreactions.

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