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1.
J Colloid Interface Sci ; 667: 385-392, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38640657

RESUMEN

Introducing the appropriate vacancies to augment the active sites and improve the electrochemical kinetics while maintaining high cyclability is a major challenge for its widespread application in electrochemical energy storage. Here, core-shell structured Bi2S3@C with sulfur vacancies was prepared by hydrothermal method and one-step carbonization/sulfuration process, which significantly improves the intrinsic electrical conductivity and ion transport efficiency of Bi2S3. Additionally, the uniform protective carbon layer around surface of composite maintains structural stability and effectively alleviates volume expansion during alloying/dealloying. As a result, the BSC-500 anode exhibits a brilliant reversible capacity of 636 mAh/g at 0.2 A/g and a long-term stable capacity of 524 mAh/g for 500 cycles at a high current density of 3 A/g in lithium-ion batteries. In addition, the assembled Bi2S3@C//LiCoO2 full cell delivered a capacity of 184 mAh/g at 1 A/g and excellent cyclability (125 mAh/g after 1000 cycles). The proposed strategy of combining sulfur vacancies with a core-shell structure to improve the electrochemical kinetics of Bi2S3 in lithium-ion batteries off the prospect for practical applications of transition metal sulfide anodes.

2.
Nano Lett ; 24(11): 3361-3368, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38446607

RESUMEN

For the first time, a series of MXene (Ti3C2Tx)/Bi2WO6 Schottky junction piezocatalysts were constructed, and the piezocatalytic hydrogen evolution activity was explored. Optimal Ti3C2Tx/Bi2WO6 exhibits the highest piezocatalytic hydrogen evolution rate of 764.4 µmol g-1 h-1, which is nearly 8 times higher than that of pure Ti3C2Tx and twice as high as that of Bi2WO6. This value also surpasses that of most recently reported typical piezocatalysts. Moreover, related experimental results and density functional theory calculations reveal that Ti3C2Tx/Bi2WO6 can provide unique channels for efficient electron transfer, enhance piezoelectric properties, optimize the adsorption Gibbs free energy of water, reduce activation energy for hydrogen atoms, endow robust separation capacity of charge carrier, and restrict the electron-hole recombination rate, thus significantly promoting the efficiency of hydrogen evolution reaction. Ultimately, we have unraveled an innovative piezocatalytic mechanism. This work broadens the scope of MXene materials in a sustainable energy piezocatalysis application.

3.
Nanoscale ; 16(15): 7660-7669, 2024 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-38529700

RESUMEN

The development of layered metal sulfides with stable structure and accessible active sites is of great importance for sodium-ion batteries (SIBs). Herein, a simple liquid-mixing method is elaborately designed to immobilize WS2 nanoflakes on N-doped carbon (NC), then further coat carbon to produce WS2/NC@C. In the formation process of this composite, the presence of NC not only avoids the overlap and improves the dispersion of WS2 nanoflakes, but also creates a connection network for charge transfer, where the wrapped carbon provides a stable chemical and electrochemical reaction interface. Thus, the composite of WS2/NC@C exhibits the desired Na+ storage capacity as anticipated. The reversible capacity reaches the high value of 369.8 mA h g-1 at 0.2 A g-1 after 200 cycles, while excellent rate performances and cycle life are also acquired in that capacity values of 256.7 and 219.6 mA h g-1 at 1 and 5 A g-1 are preserved after 1000 cycles, respectively. In addition, the assembled sodium-ion hybrid capacitors (SIHCs, AC//WS2/NC@C) exhibit an energy/power density of 68 W h kg-1 at 64 W kg-1, and capacity retention of 82.9% at 1 A g-1 after 2000 cycles. The study provides insight into developing layered metal sulfides with eminent performance of Na+ storage.

4.
Inorg Chem ; 63(7): 3467-3476, 2024 Feb 19.
Artículo en Inglés | MEDLINE | ID: mdl-38306402

RESUMEN

The energy gap and conduction band position of catalysts play crucial roles in solar-to-hydrogen (STH) transformation technology. Unfortunately, although an increase in the conduction band position can effectively promote the photoreduction capacity of the photocatalyst, it will inevitably widen the band gap, thus reducing the light-absorption scale. It seems that there is a contradiction between the reduction of band gap and the improvement of conduction band position, which is that "You can't have your cake and eat it too." Herein, an ultrasimple molecular adsorption strategy was engineered by adsorbing hydrazine hydrate on the surface of TiO2. The theoretical and experimental results indicated that the strong electron-donating effect of amino groups in hydrazine hydrate can promote the redistribution of photogenerated electrons and form surface electron networks on the surface of TiO2 photocatalysts, which can bend the conduction band upward and significantly improve its photoreduction ability. Besides, the adsorption of -NH2 can narrow the band gap width of TiO2 and promote the separation efficiency of photogenerated carriers. More interestingly, it can also effectively enhance the adsorption of H2O and H+, thus greatly elevating the STH efficiency. The STH rate of the as-prepared T-N-3 can be increased by ≈530%. This work sheds light on a new approach for resolving the contradiction between photoreduction and light absorption capabilities to effectively enhance photocatalytic performance.

5.
Chem Commun (Camb) ; 60(14): 1892-1895, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38277152

RESUMEN

Cerium-doped bismuth oxybromide (1%, 5% and 10% Ce-BiOBr) piezocatalysts were synthesized. The piezocatalytic activity was efficiently regulated by defect and morphology engineering. Among them, the 5% Ce-BiOBr exhibits the highest piezocatalytic hydrogen production property with an evolution rate of 1147.6 µmol g-1 h-1, nearly twice that of the original BiOBr. Additionally, the MO dye degradation efficiency of 5% Ce-BiOBr reaches 91.9% within 60 min, with a higher reaction kinetic constant (0.0376 min-1) that was 6.1 times larger than that of pure BiOBr. These outstanding performances of 5% Ce-BiOBr surpass those of most other piezocatalytic material systems.

6.
Inorg Chem ; 63(5): 2803-2813, 2024 Feb 05.
Artículo en Inglés | MEDLINE | ID: mdl-38243893

RESUMEN

Developing low-cost electrocatalysts with excellent activity and durability in urea-assisted water splitting is urgently needed in order to achieve sustainable hydrogen production. Herein, we in situ synthesized a robust coupled heterostructured electrocatalyst (CoP/MoO2) on a nickel foam (NF) substrate and explored its electrocatalytic performances in the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and urea oxidation reaction (UOR). The overpotential of CoP/MoO2/NF is found to be only 11 mV at 10 mA cm-2 during the HER process, which is significantly lower than that of commercial Pt/C. Meanwhile, the UOR catalytic performance of CoP/MoO2/NF indicates fast reaction kinetics, along with a considerable low driving potential (1.26 V) compared to that of the OER (1.51 V). In situ and ex situ techniques demonstrate that these excellent electrocatalytic properties are mainly ascribed to the effective synergistic coupled effect and strong electronic interactions between single-component CoP and MoO2, which can tune electronic states of Co and Mo, expose more active sites, enhance intrinsic catalytic activity, and accelerate charge transfer. Moreover, when used in electrochemical overall water splitting and urea-assisted water electrolysis, CoP/MoO2/NF can reach a current density of 10 mA cm-2 at only 1.46 and 1.32 V. This outperforms Pt/C||RuO2 and numerous nonprecious metal electrocatalysts and maintains a stable long-term electrolytic operation for 84 h. This work provides a promising pathway for the development of efficient catalysts during urea-assisted water electrolysis for hydrogen production.

7.
J Colloid Interface Sci ; 656: 545-555, 2024 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-38011773

RESUMEN

The ingenious architectural structural engineering is extensively identified as a cogent means for facilitating the electrochemical properties of conversion-type anode materials for sodium-ion storage. Herein, a delicate, scalable and controllable solvent-free strategy is proposed to synthesize ultrafine Mn2O3 quantum dots embedded into N-doped carbon to generate two-dimensional (2D) composites (MNC) with robust interfacial heterostructural interactions for high sodium ion storage and fast reaction kinetics, which averts the use of solvents and environmental pollution, greatly reduces time and production costs. The introduction of metallic Mn species simultaneously achieves the construction of ultrafine Mn2O3 quantum dots and strong interfacial heterostructural COMn bonds between metal species and 2D N-doped carbon matrix. The synergistic effect of the formation of oxide quantum dots, the combination of 2D N-doped carbon and the construction of robust interfacial interactions provides the stable electrode structure, fast reaction kinetics and high electrochemical storage capability of anode materials. Hence, MNC composites in SIBs convey remarkable reversible rate capability. Its superior capacity reaches 215 mAh g-1 for 50 cycles at 0.2 A g-1 and 155 mAh g-1 for 1000 cycles at a high current density of 5 A g-1, which shows good long-term stability. The assembled sodium-ion hybrid capacitors (SIHCs) device delivers outstanding energy density of 138 Wh kg-1 at a power density of 126 W kg-1 and 98% capacity retention after 2000 cycles at 2 A g-1, and tremendous capability for practical applications (69 LEDs can be easily lighted). This work not merely offers guidance for the rational interfacial engineering design of high-capacity Mn-based electrode materials in a feasible and scalable solvent-free tactics for Na+ storage, but also broadens the routes for projecting a better electrode material for other battery systems.

8.
Small ; : e2307771, 2023 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-38155151

RESUMEN

Constructing quantum dot-scale metal sulfides with defects and strongly coupled with carbon is significant for advanced sodium-ion batteries (SIBs). Herein, Se substituted V3 S4 quantum dots with anionic defects confined in nitrogen-doped carbon matrix (V3 S4-x Sex /NC) are fabricated. Introducing element Se into V3 S4 crystal expands the interlayer distance of V3 S4 , and triggers anionic defects, which can facilitate Na+ diffusions and act as active sites for Na+ storage. Meanwhile, the quantum dots tightly encapsulated by conductive carbon framework improve the stability and conductivity of the electrode. Theoretical calculations also unveil that the presence of Se enhances the conductivity and Na+ adsorption ability of V3 S4-x Sex . These properties contribute to the V3 S4-x Sex /NC with high specific capacity of 447 mAh g-1 at 0.2 A g-1 , and prominent rate and cyclic performance with 504 mAh g-1 after 1000 cycles at 10 A g-1 . The sodium-ion hybrid capacitors (SIHCs) with V3 S4-x Sex /NC anode and activated carbon cathode can achieve high energy/power density (maximum 144 Wh kg-1 /5960 W kg-1 ), capacity retention ratio of 71% after 4000 cycles at 2 A g-1 . This work not only synthesizes V3 S4-x Sex /NC, but also provides a promising opportunity for designing quantum dots and utilizing defects to improve the electrochemical properties.

9.
Inorg Chem ; 62(37): 15249-15257, 2023 Sep 18.
Artículo en Inglés | MEDLINE | ID: mdl-37676295

RESUMEN

Constructing heterojunctions with strong interfacial interactions can accelerate the transfer and separation of photogenerated charge carriers. However, finding a simple strategy to construct tightly connected heterojunctions remains a major challenge. In this work, AgBr/BiOBr S-scheme heterojunctions were designed via a straightforward co-anionic strategy without using a solvent. The experimental results indicate that the AgBr/BiOBr heterojunction with a close contact interface can extend the use of visible light, accelerate the separation, and induce the transfer of photoelectrons and holes while maintaining an excellent redox capacity. Undoubtedly, the photocatalytic reduction rate of carbon dioxide to carbon monoxide by 1.0 AgBr/BiOBr is 87.73 µmol·g-1·h-1 (quantum efficiency is 0.57%), which is 12.15 times and 4.45 times higher than that of pure AgBr and BiOBr, respectively. The present work provides insights into a simple strategy for the preparation of strongly interacting interfacial heterojunctions for photocatalytic CO2 reduction.

10.
J Colloid Interface Sci ; 646: 34-42, 2023 Sep 15.
Artículo en Inglés | MEDLINE | ID: mdl-37182257

RESUMEN

Developing anode materials with high reversible capacity, fast redox kinetics, and stable cycling life for Na+ storage remains a great challenge. Herein, the VO2 nanobelts with oxygen vacancies supported on nitrogen-doped carbon nanosheets (VO2-x/NC) were developed. Benefitting from the enhanced electrical conductivity, the accelerated kinetics, the increased active sites as well as the constructed 2D heterostructure, the VO2-x/NC delivered extraordinary Na+ storage performance in half/full battery. Theoretical calculations (DFT) demonstrated that oxygen vacancies could regulate the adsorption ability for Na+, enhance electronic conductivity, as well as achieve rapid and reversible Na+ adsorption/desorption. The VO2-x/NC exhibited high Na+ storage capacity of 270 mAh g-1 at 0.2 A g-1, and impressive cyclic stability with 258 mAh g-1 after 1800 cycles at 10 A g-1. The assembled sodium-ion hybrid capacitors (SIHCs) could achieve maximum energy density/power output of 122 Wh kg-1/9985 W kg-1, ultralong cycling life with 88.4% capacity retention after 25,000 cycles at 2 A g-1, and practical applications (55 LEDs could be actuated for 10 min), promising to be utilized in a practicable Na+ storage.

11.
Inorg Chem ; 62(16): 6428-6438, 2023 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-37032488

RESUMEN

Developing high-efficiency, low-cost, and earth-abundant electrocatalysts toward the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) is highly desirable for boosting the energy efficiency of water splitting. Herein, we adopted an interfacial engineering strategy to enhance the overall water splitting (OWS) activity via constructing a bifunctional OER/HER electrocatalyst combining MoS2-Ni3S2 with NiFe layered double hydroxide (NiFe-LDH) on a nickel foam substrate. The NiFe-LDH/MoS2-Ni3S2/NF electrocatalyst delivers superior OER/HER activity and stability, such as low overpotentials (220 and 79 mV for OER and HER at current densities of 50 and 10 mA cm-2, respectively) and a low Tafel slope. This excellent electrocatalytic performance mainly benefits from the electronic structure modulation and synergistic effects between NiFe-LDH and MoS2-Ni3S2, which provides a high electrochemical activity area, more active sites, and strong electron interaction. Furthermore, the assembly of NiFe-LDH/MoS2-Ni3S2/NF into a two-electrode system only requires an ultra-low cell voltage of 1.50 V at a current density of 10 mA cm-2 and exhibits outstanding stability with a decay of current density of only 2.11% @50 mA cm-2 after 50 h, which is far superior to numerous other reported transition metal NiFe-LDH and MoS2-Ni3S2-based as well as RuO2||Pt-C electrocatalysts. This research highlights the rational design of heterostructures to efficiently advance electrocatalysis for water splitting applications.

12.
Inorg Chem ; 62(8): 3532-3540, 2023 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-36791254

RESUMEN

Electrocatalytic water splitting is still circuitous and controversial because of the lack of highly active electrocatalysts to decrease the overpotential. Herein, we report a feasible method for constructing heterojunctions of MnO2-Co3O4 nanosheets on Co@NCNT support surfaces (MnO2-Co3O4/Co@NCNT) by spontaneous redox reactions. Experimental results indicate that Co embedded in Co@NCNT can be used as the carbon support and anchoring sites for heterojunctions, thus exposing a large number of active sites, adjusting the surface electronic structure, changing the OER rate-determining step of the catalyst, and reducing the reaction energy barrier. Besides, the in situ formation of MnO2-Co3O4 nanosheets on Co@NCNT inhibits the loss and aggregation of the catalyst, leading to robust structural stability. Therefore, the synergistic effects of these factors provide multi-functional active sites to enhance the intrinsic activity and achieve maximum catalytic performances. To deliver a current density of 10 mA cm-2, the catalyst of MnO2-Co3O4/Co@NCNT achieves an overpotential (η) of 303 mV in 1.0 M KOH media for OER. This simple redox strategy can be easily extended to prepare other ultrathin transition-metal oxide heterojunctions, which could be applied not only for water splitting but also for other energy conversion and storage technologies.

13.
J Colloid Interface Sci ; 639: 343-354, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-36812851

RESUMEN

Piezocatalysis as an emerging technology is broadly applied in hydrogen evolution and organic pollutants degradation aspects. However, the dissatisfactory piezocatalytic activity is a severe bottleneck for its practical applications. In this work, CdS/BiOCl S-scheme heterojunction piezocatalysts were constructed and explored the performances of piezocatalytic hydrogen (H2) evolution and organic pollutants degradation (methylene orange, rhodamine B and tetracycline hydrochloride) under strain by ultrasonic vibration. Interestingly, CdS/BiOCl presents a volcano-type relationship between catalytic activity and CdS contents, namely firstly increases and then decreases with the increase of CdS content. Optimal 20 % CdS/BiOCl endows superior piezocatalytic H2 generation rate of 1048.2 µmol g-1h-1 in methanol solution, which is 2.3 and 3.4 times higher than that of pure BiOCl and CdS, respectively. This value is also much higher than the recently reported Bi-based and most of other typical piezocatalysts. Meanwhile, 5 % CdS/BiOCl delivers the highest reaction kinetics rate constant and degradation rate toward various pollutants compared with other catalysts, which also exceeds that of the previously numerous results. Improved catalytic capacity of CdS/BiOCl is mainly ascribed to the construction of S-scheme heterojunction for enhancing the redox capacity as well as inducing more effective charge carriers separation and transfer. Moreover, S-scheme charge transfer mechanism is demonstrated via electron paramagnetic resonance and Quasi-In-situ X-ray photoelectron spectroscopy measurements. Eventually, a novel piezocatalytic mechanism of CdS/BiOCl S-scheme heterojunction has been proposed. This research develops a novel pathway for designing highly efficient piezocatalysts and provides a deeper understanding in construction of Bi-based S-scheme heterojunction catalysts for energy conservation and wastewater disposal applications.

14.
Small ; 19(16): e2207214, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36670333

RESUMEN

The exploitation of electrode materials with ability to balance capacity and kinetics between cathode and anode is a challenge for sodium-ion hybrid capacitors (SIHCs). Mn-based anode materials are limited by poor electrical conductivity, sluggish reaction kinetics, large volume variation, weak cycling stability, and inferior reversible capacity. Herein, MnS nanocubes encapsulated in S-doped porous carbon matrix (MSC) with strong sulfur-bridged bond interactions (CSMn) are successfully synthesized by solvent-free tactics. The CSMn bonds generated between MnS and carbon significantly inhibit the aggregation of nanostructural MnS cubes, restrict the volume expansion, and stabilize the nanostructure, which improves the Na+ storage reversibility and stability. Moreover, S-doped porous carbon enhances the electrical conductivity and electrons/ions diffusion rate, which boosts a fast kinetic reaction. As expected, MSC anode presents an outstanding reversible capacity of 600 mAh g-1 at 0.2 A g-1 and a long-term stable capacity of 357 mAh g-1 for 1000 cycles at a high current density of 10 A g-1 in sodium-ion batteries (SIBs). The as-assembled SIHCs deliver a high energy density of 109 W h kg-1 and a high power output of 98 W kg-1 , with 88% capacity retention at 2 A g-1 after 2000 cycles and practical applications (55 LEDs can be lighted for 10 min).

15.
J Colloid Interface Sci ; 626: 475-485, 2022 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-35803146

RESUMEN

Highly efficient oxygen reduction and oxygen evolution reactions have the critical role in the practical application of zinc-air batteries. Herein, doping engineering strategy has been adopted by construction of Se/Fe-doped in Co3O4/N-doped carbon nanosheets (denoted as Se/Fe-Co3O4/N-CNs) catalyst for boosting oxygen electrocatalytic activity. The achieved Se/Fe-Co3O4/N-CNs catalyst presents high-performances electrocatalytic characteristics, which exhibits a small overpotential gap (0.79 V), excellent oxygen evolution reaction activity with a small overpotential of 361 mV and a low Tafel slope of 57.3 mV dec-1 at 10 mA cm-2 as well as excellent oxygen reduction reaction activity with a large half-wave potential of 0.8 V, also surpassing the majority of reported Co3O4-based electrocatalysts. The outstanding catalytic performances are benefiting from the contributions between Se/Fe doping engineering and N-doped carbon nanosheets optimizing the electronic structure of Co species, endowing more active sites, enhancing the intrinsic catalytic activity and accelerating charge transfer rate for oxygen electrocatalytic process. Particularly, the as-fabricated zinc-air batteries with Se/Fe-Co3O4/N-CNs as air cathode presents a high open circuit potential of 1.41 V, a prominent highly efficient peak power density of 141.3 mW cm-2, a high specific capacity of 765.6 mAh g-1 and energy density 861.3 Wh kg-1 at current density of 10 mA cm-2 as well as an excellent cycling stability, which are exceeding the commercial Pt/C-RuO2 based zinc-air batteries. This work lays a foundation for design and development of high-performance bifunctional cobalt-based electrocatalysts for rechargeable metal-air batteries application.

16.
Inorg Chem ; 61(21): 8217-8225, 2022 May 30.
Artículo en Inglés | MEDLINE | ID: mdl-35584061

RESUMEN

Defects play a vital role in improving photocatalytic performance. However, the specific influence mechanism of sulfur defects (DSS) on sulfide photocatalytic performance and stability is still unclear. In this work, an ingenious solvent-free self-overflow strategy is designed to introduce DSS into ZnS nanoparticles and explore the specific promotion mechanism of photocatalytic performance and photostability. The results indicate that the introduced DSS in ZnS nanoparticles can simultaneously boost the photocatalytic hydrogen production (PHE) performance and photostability of ZnS: the PHE rate of the defective ZnS can increase up to 21350.23 µmol·h-1·g-1, which is roughly 4.7 times higher than that of pristine ZnS. Both experiments and theoretical calculationsshow that the enhanced photocatalytic performance could be attributed to the change of energy band position after introducing DSS. Specifically, the introduction of DSS can raise the conduction band (CB) position of ZnS to enhance the reducing ability of photogenerated electrons. Besides, the valence band (VB) position can also be raised to boost the light absorption ability of ZnS and restrain the photocorrosion by weakening the oxidation capacity of the photogenerated holes. The ingenious strategy and interesting mechanism in this job provide a simple artful tactic to fabricate other defective sulfide photocatalysts and open up a particular path to promote the photostability of the photocatalysts.

17.
J Colloid Interface Sci ; 612: 111-120, 2022 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-34983011

RESUMEN

Surface modification by hydrophilic functional group have a tremendous influence on the catalytic activity of photocatalyst, however, there are few reports on improving piezoelectric catalytic performance through surface functionalization. Herein, OH-modified SrTiO3 was successfully obtained via a novel low-temperature solid-state precursor method and employed as a catalyst for photocatalytic, piezocatalytic and piezo-photocatalytic hydrogen production. Thanks to the super hydrophilic that is facilitating the contact of catalyst and water molecular and the more oxygen vacancies that can promote electron-hole separation, the photocatalytic, piezocatalytic and piezo-photocatalytic hydrogen generation of OH-modified SrTiO3 (OH-STO) is about two times higher than pristine SrTiO3 (STO). It is worth mentioning that the optimal piezo-photocatalytic hydrogen evolution rate of OH-STO (701.2 µmol h-1 g-1) is 5.3 times higher than the photocatalytic hydrogen evolution process of STO. This study presents a low-energy approach to the rational design of functional group modification nanomaterials that possess excellent piezo-photocatalytic performance.

18.
Small ; 17(52): e2104656, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34741432

RESUMEN

Simultaneous boosting electrochemical methanol oxidation reaction (MOR) for direct methanol fuel cells and production of hydrogen is meaningful but challenging. Herein, a sea urchin-shaped cobalt-embedded N-doped carbon nanotubes (Co@NCNT) encapsulated CoPt3 @Co2 P heterojunction (CoPt3 @Co2 P/Co@NCNT) is fabricated. Theoretical calculations confirm that electrons at the interfaces transfer from CoPt3 to Co2 P, where electron hole region on CoPt3 is beneficial to improving the MOR activity, whereas accumulation region on Co2 P favors to the optimization of H2 O and H* absorption energies for hydrogen evolution reaction (HER). Benefitting from its interfacial electronic reconfiguration, the CoPt3 @Co2 P/Co@NCNT heterojunction exhibits excellent electrocatalytic performances for MOR and HER, in which the mass activity (2981 mA mgPt -1 ) for MOR is 14.2 times than that of Pt/C (20%), and the smallest overpotentials only requires 19 mV to deliver a current density of 10 mA cm-2 for HER. Moreover, the electrolyzer employing CoPt3 @Co2 P/Co@NCNT for anodic MOR and cathodic H2 production only requires a low voltage of 1.43 V at 10 mA cm-2 with impressive long-life cycling stability, which is obviously better than that of commercial Pt/C//RuO2 . This study offers a novel strategy for other organics oxidation reaction coupled with HER catalyzed production of hydrogen.

19.
J Colloid Interface Sci ; 588: 670-679, 2021 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-33267952

RESUMEN

Interfacial modification and band modulation to narrow the band gap and improve light-harvesting ability of TiO2 are promising strategies to dramatically promote photocatalytic activity. Herein, efficient Co(OH)2-TiO2 nanocomposites were reasonably designed and constructed by a facile room temperature solid-state synthetic strategy for interfacial modification and matched band gap to achieve the conversion of solar energy to hydrogen. Modifying transition metal hydroxide Co(OH)2 on commercial TiO2 can effectively narrow the band gap and accelerate the separation and migration of photo-induced carriers, which will extend light absorption range and facilitate more electrons transferring to the surface of photocatalyst, therefore the reducibility of photocatalysts is enhanced. The modified photocatalyst exhibits high photocatalytic hydrogen evolution activity and stability. Specifically, the obtained TCO-0.6 shows excellent photocatalytic hydrogen evolution rate of 21343.01 µmol g-1 and is 23 times superior to commercial TiO2. This work not only emphasizes a facile strategy for interfacial modification and band modulation under mild condition, but also provides a novel avenue for improving the performance of photocatalytic hydrogen evolution.

20.
J Colloid Interface Sci ; 577: 290-299, 2020 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-32485412

RESUMEN

The piezoelectric zinc oxides with different morphology (ZnO nanoparticles and nanorods, hereafter abbreviated as ZnO NPs and NRs) are successfully synthesized using facile, green and harmless solid-state chemistry method at room temperature. The piezocatalytic activity of zinc oxide towards methylene blue (MB) of organic pollutants degradation has been explored under ultrasonic vibration. The ZnO NRs exhibit effectively enhanced piezocatalytic performance towards degradation dye compared with the ZnO NPs. In particular, the piezocatalytic decolorization ratio of MB solution is up to ~38% in ZnO NRs under 120 min, ~ 99% under 5.5 h and show good recycling utilization characteristics, indicating great potential for dye wastewater decolorization treatment. The main oxidizing hydroxyl radical (OH) and superoxide radicals (O2-) of the piezocatalytic reactions are confirmed and the production of piezocatalytic degradation process induced polarization electric charges. Moreover, we investigate the relationship between morphology and piezoelectric potential based on the finite element method for ZnO NPs and NRs, which further clarify the enhanced piezocatalytic activity and insight into piezocatalytic mechanism. This work offers a novel strategy towards wastewater decontamination applications and further understanding the relationship between piezocatalysis, morphology, and piezocatalytic mechanism in piezoelectric materials.

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