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1.
Nat Commun ; 15(1): 2290, 2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38480686

RESUMEN

The precise structural integration of single-atom and high-entropy-alloy features for energy electrocatalysis is highly appealing for energy conversion, yet remains a grand challenge. Herein, we report a class of single-atom Mo-tailored PdPtNiCuZn high-entropy-alloy nanosheets with dilute Pt-Pt ensembles and intrinsic tensile strain (Mo1-PdPtNiCuZn) as efficient electrocatalysts for enhancing the methanol oxidation reaction catalysis. The as-made Mo1-PdPtNiCuZn delivers an extraordinary mass activity of 24.55 A mgPt-1 and 11.62 A mgPd+Pt-1, along with impressive long-term durability. The planted oxophilic Mo single atoms as promoters modify the electronic structure of isolated Pt sites in the high-entropy-alloy host, suppressing the formation of CO adsorbates and steering the reaction towards the formate pathway. Meanwhile, Mo promoters and tensile strain synergistically optimize the adsorption behaviour of intermediates to achieve a more energetically favourable pathway and minimize the methanol oxidation reaction barrier. This work advances the design of atomically precise catalytic sites by creating a new paradigm of single atom-tailored high-entropy alloys, opening an encouraging pathway to the design of CO-tolerance electrocatalysts.

2.
J Environ Manage ; 353: 120225, 2024 Feb 27.
Artículo en Inglés | MEDLINE | ID: mdl-38330837

RESUMEN

China's growing demand for bulk chemicals and concerns regarding energy security are scaling up coal-to-olefins (CTO) production. Three generations of independent dimethyl ether/methanol-to-olefins technologies have been successively launched with greatly improved production efficiencies. However, to date, widespread concerns regarding the intensive environmental impacts and potential economic risks have not been addressed in the context of this industrialization. Here we show that, through the technological progress from the first to the third generation, life cycle energy consumption, water consumption, and carbon emissions can be reduced to 119.5 GJ/t, 27.6 t/t, and 9.1 t CO2-eq/t, respectively, and human health damage, ecosystem quality damage, and resource scarcity impacts can be decreased by 40.5 %, 50.1 %, and 16.4 %, respectively. This is accompanied by an excellent performance in terms of production cost, net present value, and internal return rate at 792.5 USD/t, 173.4 USD/t, and 19.4 %, respectively. Substantial environmental and economic benefits can be gained by coupling renewables in the form of using green hydrogen from solar and wind power to synthesize methanol. Particularly, life cycle carbon emissions and resource scarcity impacts are reduced by 23.4 % and 22.4 %, respectively, exceeding the reduction in technological progress. However, coupling renewables increases the life cycle energy consumption to 154.5 GJ/t, counteracting the benefits of technological progress. Our results highlight the importance of technological progress and coupled renewables for enhancing the sustainability of the CTO industry.


Asunto(s)
Alquenos , Carbón Mineral , Humanos , Ecosistema , Metanol , Desarrollo Económico , Carbono/análisis , Dióxido de Carbono/análisis , China
3.
J Am Chem Soc ; 146(7): 4433-4443, 2024 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-38329948

RESUMEN

Potassium-sulfur (K-S) batteries are severely limited by the sluggish kinetics of the solid-phase conversion of K2S3/K2S2 to K2S, the rate-determining and performance-governing step, which urgently requires a cathode with facilitated sulfur accommodation and improved catalytic efficiency. To this end, we leverage the orbital-coupling approach and herein report a strong d-π coupling catalytic configuration of single-atom Co anchored between two alkynyls of graphdiyne (Co-GDY). The d-π orbital coupling of the Co-C4 moiety fully redistributes electrons two-dimensionally across the GDY, and as a result, drastically accelerates the solid-phase K2S3/K2S2 to K2S conversion and enhances the adsorption of sulfur species. Applied as the cathode, the S/Co-GDY delivered a record-high rate performance of 496.0 mAh g-1 at 5 A g-1 in K-S batteries. In situ and ex situ characterizations coupling density functional theory (DFT) calculations rationalize how the strong d-π orbital coupling of Co-C4 configuration promotes the reversible solid-state transformation kinetics of potassium polysulfide for high-performance K-S batteries.

4.
J Am Chem Soc ; 146(4): 2339-2344, 2024 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-38237055

RESUMEN

Li-O2 batteries (LOBs) are considered as one of the most promising energy storage devices due to their ultrahigh theoretical energy density, yet they face the critical issues of sluggish cathode redox kinetics during the discharge and charge processes. Here we report a direct synthetic strategy to fabricate a single-atom alloy catalyst in which single-atom Pt is precisely dispersed in ultrathin Pd hexagonal nanoplates (Pt1Pd). The LOB with the Pt1Pd cathode demonstrates an ultralow overpotential of 0.69 V at 0.5 A g-1 and negligible activity loss over 600 h. Density functional theory calculations show that Pt1Pd can promote the activation of the O2/Li2O2 redox couple due to the electron localization caused by the single Pt atom, thereby lowering the energy barriers for the oxygen reduction and oxygen evolution reactions. Our strategy for designing single-atom alloy cathodic catalysts can address the sluggish oxygen redox kinetics in LOBs and other energy storage/conversion devices.

5.
Adv Mater ; 36(8): e2306292, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37723937

RESUMEN

Nanozymes, as one of the most efficient reactive oxygen species (ROS)-scavenging biomaterials, are receiving wide attention in promoting diabetic wound healing. Despite recent attempts at improving the catalytic efficiency of Pt-based nanozymes (e.g., PtCu, one of the best systems), they still display quite limited ROS scavenging capacity and ROS-dependent antibacterial effects on bacteria or immunocytes, which leads to uncontrolled and poor diabetic wound healing. Hence, a new class of multifunctional PtCuTe nanosheets with excellent catalytic, ROS-independent antibacterial, proangiogenic, anti-inflammatory, and immuno-modulatory properties for boosting the diabetic wound healing, is reported. The PtCuTe nanosheets show stronger ROS scavenging capacity and better antibacterial effects than PtCu. It is also revealed that the PtCuTe can enhance vascular tube formation, stimulate macrophage polarization toward the M2 phenotype and improve fibroblast mobility, outperforming conventional PtCu. Moreover, PtCuTe promotes crosstalk between different cell types to form a positive feedback loop. Consequently, PtCuTe stimulates a proregenerative environment with relevant cell populations to ensure normal tissue repair. Utilizing a diabetic mouse model, it is demonstrated that PtCuTe significantly facilitated the regeneration of highly vascularized skin, with the percentage of wound closure being over 90% on the 8th day, which is the best among the reported comparable multifunctional biomaterials.


Asunto(s)
Diabetes Mellitus , Cicatrización de Heridas , Animales , Ratones , Especies Reactivas de Oxígeno , Piel , Antibacterianos/farmacología , Antibacterianos/uso terapéutico , Materiales Biocompatibles/farmacología , Hidrogeles
6.
Small ; 20(7): e2305817, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37814379

RESUMEN

Complete ethanol oxidation reaction (EOR) in C1 pathway with 12 transferred electrons is highly desirable yet challenging in direct ethanol fuel cells. Herein, PtRh jagged nanowires synthesized via a simple wet-chemical approach exhibit exceptional EOR mass activity of 1.63 A mgPt-1 and specific activity of 4.07 mA cm-2 , 3.62-fold and 4.28-folds increments relative to Pt/C, respectively. High proportions of 69.33% and 73.42% of initial activity are also retained after chronoamperometric test (80 000 s) and 1500 consecutive potential cycles, respectively. More importantly, it is found that PtRh jagged nanowires possess superb anti-CO poisoning capability. Combining X-ray absorption spectroscopy, X-ray photoelectron spectroscopy as well as density functional theory calculations unveil that the remarkable catalytic activity and CO tolerance stem from both the Rh-induced electronic effect and geometric effect (manifested by shortened Pt─Pt bond length and shrinkage of lattice constants), which facilitates EOR catalysis in C1 pathway and improves reaction kinetics by reducing energy barriers of rate-determining steps (such as *CO → *COOH). The C1 pathway efficiency of PtRh jagged nanowires is further verified by the high intensity of CO2 relative to CH3 COOH/CH3 CHO in infrared reflection absorption spectroscopy.

7.
Chem Rev ; 123(22): 12507-12593, 2023 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-37910391

RESUMEN

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic nanocrystals have been known to show distinct properties compared to their disordered counterparts, and been long explored for functional improvements. Tremendous progresses have been made in the past few years, with notable trend of more precise engineering down to an atomic level and the investigation transferring into more practical membrane electrode assembly (MEA), which motivates this timely review. After addressing the basic thermodynamic and kinetic fundamentals, we discuss classic and latest synthetic strategies that enable not only the formation of intermetallic phase but also the rational control of other catalysis-determinant structural parameters, such as size and morphology. We also demonstrate the emerging intermetallic nanomaterials for potentially further advancement in energy electrocatalysis. Then, we discuss the state-of-the-art characterizations and representative intermetallic electrocatalysts with emphasis on oxygen reduction reaction evaluated in a MEA setup. We summarize this review by laying out existing challenges and offering perspective on future research directions toward practicing intermetallic electrocatalysts for energy conversions.

8.
Animals (Basel) ; 13(22)2023 Nov 13.
Artículo en Inglés | MEDLINE | ID: mdl-38003119

RESUMEN

Eimeria tenella rhoptry protein has the properties of a protective antigen. EtROP27 is a pathogenic gene that is detected via a transcriptome, but its expression pattern, immunogenicity, and potency are unknown. Therefore, a gene segment of EtROP27 was amplified and transplanted into the pET28a prokaryotic vector for the expression of the recombinant protein, and it subsequently purified for the generation of a polyclonal antibody. Then, RT-PCR and Western blotting were performed to understand the expression pattern of EtROP27. Subsequently, animal experiments were conducted to evaluate the immunoprotective effect of the recombinant protein with different immunizing doses (50, 100, and 150 µg). The results showed that the expression of EtROP27 gradually increased with the prolongation of infection time, reaching the highest level at 96 h and then decreasing. Additionally, EtROP27 is a natural antigen of coccidia that can stimulate the body to produce high levels of IgY. As with recombinant protein vaccines, the results of immune protection evaluation tests showed that the average weight gain rates of the immune challenge groups were significantly higher than that of the challenged control group, and their average lesion scores were significantly lower than that of the challenged control group. Furthermore, the oocyst excretion decreased by 81.25%, 86.21%, and 80.01%, and the anticoccidial index was 159.45, 171.47, and 166.75, respectively, for these groups. EtROP27 is a promising antigen gene candidate for the development of a coccidiosis vaccine.

9.
J Am Chem Soc ; 145(39): 21432-21441, 2023 Oct 04.
Artículo en Inglés | MEDLINE | ID: mdl-37728051

RESUMEN

Although dispersing Pt atomic clusters (ACs) on a conducting support is a promising way to minimize the Pt amount required in hydrogen evolution reaction (HER), the catalytic mass activity and durability of Pt ACs are often unsatisfactory for alkaline HER due to their unfavorable water dissociation and challenges in stabilizing them against agglomeration and detachment. Herein, we report a class of single-atom Cr-N4 sites with high oxophilicity interfaced with Pt ACs on mesoporous carbon for achieving a highly active and stable alkaline HER in an anion-exchange-membrane water electrolyzer (AEMWE). The as-made catalyst achieves the highest reported Pt mass activity (37.6 times higher than commercial Pt/C) and outstanding operational stability. Experimental and theoretical studies elucidate that the formation of a unique Pt-Cr quasi-covalent bonding interaction at the interface of Cr-N4 sites and Pt ACs effectively suppresses the migration and thermal vibration of Pt atoms to stabilize Pt ACs and contributes to the greatly enhanced catalytic stability. Moreover, oxophilic Cr-N4 sites adjacent to Pt ACs with favorable adsorption of hydroxyl species facilitate nearly barrierless water dissociation and thus enhance the HER activity. An AEMWE using this catalyst (with only 50 µgPt cm-2) can operate stably at an industrial-level current density of 500 mA cm-2 at 1.8 V for >100 h with a small degradation rate of 90 µV h-1.

10.
Entropy (Basel) ; 25(7)2023 Jul 12.
Artículo en Inglés | MEDLINE | ID: mdl-37509997

RESUMEN

The subject of oil price forecasting has obtained an incredible amount of interest from academics and policymakers in recent years due to the widespread impact that it has on various economic fields and markets. Thus, a novel method based on decomposition-reconstruction-ensemble for crude oil price forecasting is proposed. Based on the Complete Ensemble Empirical Mode Decomposition with Adaptive Noise (CEEMDAN) technique, in this paper we construct a recursive CEEMDAN decomposition-reconstruction-ensemble model considering the complexity traits of crude oil data. In this model, the steps of mode reconstruction, component prediction, and ensemble prediction are driven by complexity traits. For illustration and verification purposes, the West Texas Intermediate (WTI) and Brent crude oil spot prices are used as the sample data. The empirical result demonstrates that the proposed model has better prediction performance than the benchmark models. Thus, the proposed recursive CEEMDAN decomposition-reconstruction-ensemble model can be an effective tool to forecast oil price in the future.

11.
J Am Chem Soc ; 145(32): 17577-17587, 2023 Aug 16.
Artículo en Inglés | MEDLINE | ID: mdl-37253225

RESUMEN

Designing efficient and durable bifunctional catalysts for 5-hydroxymethylfurfural (HMF) oxidation reaction (HMFOR) and hydrogen evolution reaction (HER) is desirable for the co-production of biomass-upgraded chemicals and sustainable hydrogen, which is limited by the competitive adsorption of hydroxyl species (OHads) and HMF molecules. Here, we report a class of Rh-O5/Ni(Fe) atomic site on nanoporous mesh-type layered double hydroxides with atomic-scale cooperative adsorption centers for highly active and stable alkaline HMFOR and HER catalysis. A low cell voltage of 1.48 V is required to achieve 100 mA cm-2 in an integrated electrolysis system along with excellent stability (>100 h). Operando infrared and X-ray absorption spectroscopic probes unveil that HMF molecules are selectively adsorbed and activated over the single-atom Rh sites and oxidized by in situ-formed electrophilic OHads species on neighboring Ni sites. Theoretical studies further demonstrate that the strong d-d orbital coupling interactions between atomic-level Rh and surrounding Ni atoms in the special Rh-O5/Ni(Fe) structure can greatly facilitate surface electronic exchange-and-transfer capabilities with the adsorbates (OHads and HMF molecules) and intermediates for efficient HMFOR and HER. We also reveal that the Fe sites in Rh-O5/Ni(Fe) structure can promote the electrocatalytic stability of the catalyst. Our findings provide new insights into catalyst design for complex reactions involving competitive adsorptions of multiple intermediates.

12.
Adv Mater ; 35(32): e2302285, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37248040

RESUMEN

Strain engineering has been utilized as an effective approach to regulate the binding of reaction intermediates and modify catalytic behavior on noble metal nanocatalysts. However, the continuous, precise control of strain for a depiction of strain-activity correlation remains a challenge. Herein, Pd-based nanooctahedrons coated with two Ir overlayers are constructed, and subject to different postsynthetic treatments to alter the amount of H intercalated into Pd core for achieving three different surface strains (o-Pd/Ir-1.2%, o-Pd/Ir-1.7%, and o-Pd/Ir-2.1% NPs). It is demonstrated that the catalytic performances of o-Pd/Ir NPs display a volcano-shaped curve against strains toward the hydrogen evolution reaction (HER). Specifically, o-Pd/Ir-1.7% NPs exhibit superior catalytic performance with a mass activity of 9.38 A mgIr -1 at -0.02 V versus reversible hydrogen electrode, 10.8- and 18.8-fold higher than those of commercial Pt/C and Ir/C, respectively, making it one of the most active HER electrocatalysts reported to date. Density function theory calculations verify that the moderate tensile strain on Ir(111) surfaces plays a pivotal role in optimizing the H binding energy. This work highlights a new strategy for precise control over the surface strain of nanocrystals for more efficient electrocatalysis.

13.
Nanoscale ; 15(16): 7466-7471, 2023 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-37016770

RESUMEN

Strontium ferrite nanostructures have attracted intensive interest recently due to the increasing demand for cost-effective features and good chemical corrosion resistance of magnetic materials, yet the ultrafast synthesis of strontium ferrite with desired coercivity is still experiencing a severe challenge. Herein, porous strontium ferrite foams with a coercivity up to 23.35 kOe were prepared by ultrafast in situ annealing for 1 min based on an auto-combustion strategy. The high coercivity of strontium ferrite benefits from the increasing magnetocrystalline anisotropy caused by the ion substitution and the appropriate grain size close to the critical single-domain size of strontium ferrite. In addition, this ultrafast synthesis can be extended to prepare a series of porous spinel, lanthanide-based perovskites, and their high-entropy counterpart foams. We also demonstrate that this strategy is feasible for preparing biphasic composite oxide foams. Furthermore, this work provides important guidance for the design of porous permanent magnet materials and the efficient preparation of porous oxide foam materials.

14.
J Colloid Interface Sci ; 640: 348-358, 2023 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-36867931

RESUMEN

Developing highly active methanol oxidation electrocatalysts with superior anti-CO poisoning capability remains a grand challenge. Herein, a simple strategy was employed to prepare distinctive PtFeIr jagged nanowires with Ir located at the shell and Pt/Fe located at the core. The Pt64Fe20Ir16 jagged nanowire possesses an optimal mass activity of 2.13 A mgPt-1 and specific activity of 4.25 mA cm-2, giving the catalyst a great edge over PtFe jagged nanowire (1.63 A mgPt-1 and 3.75 mA cm-2) and Pt/C (0.38 A mgPt-1 and 0.76 mA cm-2). The in-situ Fourier transform infrared (FTIR) spectroscopy and differential electrochemical mass spectrometry (DEMS) unravel the origin of extraordinary CO tolerance in terms of key reaction intermediates in the non-CO pathway. Density functional theory (DFT) calculations add to the body of evidence that the surface Ir incorporation transforms the selectivity from CO pathway to non-CO pathway. Meanwhile, the presence of Ir serves to optimize surface electronic structure with weakened CO binding strength. We believe this work will advance the understanding of methanol oxidation catalytic mechanism and provide some insight into structural design of efficient electrocatalysts.

15.
Artículo en Inglés | MEDLINE | ID: mdl-36901667

RESUMEN

Green credit is a vital instrument for promoting low-carbon transition. However, designing a reasonable development pattern and efficiently allocating limited resources has become a challenge for developing countries. The Yellow River Basin, a critical component of the low-carbon transition in China, is still in the early stages of green credit development. Most cities in this region lack green credit development plans that suit their economic conditions. This study examined the impact of green credit on carbon emission intensity and utilized a k-means clustering algorithm to categorize the green credit development patterns of 98 prefecture-level cities in the Yellow River Basin based on four static indicators and four dynamic indicators. Regression results based on city-level panel data from 2006 to 2020 demonstrated that the development of green credit in the Yellow River Basin can effectively reduce local carbon emission intensity and promote low-carbon transition. We classified the development patterns of green credit in the Yellow River Basin into five types: mechanism construction, product innovation, consumer business expansion, rapid growth, and stable growth. Moreover, we have put forward specific policy suggestions for cities with different development patterns. The design process of this green credit development patterns is characterized by its ability to achieve meaningful outcomes while relying on fewer numbers of indicators. Furthermore, this approach boasts a significant degree of explanatory power, which may assist policy makers in comprehending the underlying mechanisms of regional low-carbon governance. Our findings provide a new perspective for the study of sustainable finance.


Asunto(s)
Personal Administrativo , Ríos , Humanos , Ciudades , Algoritmos , Carbono , China , Desarrollo Económico
16.
Comput Intell Neurosci ; 2022: 1465394, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-36188678

RESUMEN

P2P lending is an important part of Internet finance, which is popular among users because of its efficiency, low cost, wide range, and ease of operation. The problem of predicting loan defaults is affected by many factors, such as the linear and nonlinear nature of the data itself and time dependence and multiple external factors, which have not been well captured in the previous work. In this paper, we propose a multiattention mechanism to capture the different effects of various time slices and various external factors on the results, introduce ARIMA and LSTM to capture the linear and nonlinear characteristics of the lending data respectively, and establish a Time Series Multiattention Prediction Model (MAT-ALSTM) based on LSTM and ARIMA. This paper uses the Lending Club dataset from the United States to prove that our model is superior to ANN, SVM, LSTM, GRU, and ARIMA models in the prediction effect of MAE, RMSE, and DA.


Asunto(s)
Aprendizaje Profundo , Internet
17.
J Am Chem Soc ; 144(23): 10582-10590, 2022 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-35652187

RESUMEN

High-entropy alloys (HEAs) are attracting intensive attention due to their broad compositional tunability and interesting catalytic properties. However, precisely shaping the HEAs into suprathin low-dimensional nanostructures for achieving diverse applications remains an enormous challenge owing to their intrinsic thermodynamic instability. Herein we propose a new and general low-temperature method for incorporating up to eight metallic elements into one single-phase subnanometer ribbon to achieve the thinnest HEA metal materials in the world. We experimentally demonstrate that synthetic processes for suprathin HEA subnanometer ribbons (SNRs) include (1) different metal atom nucleation via galvanic exchange reaction between different metal precursors and Ag nanowire template, (2) co-reduction of different metal precursors on nanowire template, and (3) the removal of the inner Ag core. Density functional theory (DFT) calculations reveal that the crystallization and stabilization of HEA SNRs strongly depend on the "highly dynamic" Ag from the template, and the crystallization levels of HEA subnanometer ribbons are closely correlated with the concentration of Pt and Pd. We demonstrate that the present synthetic method enables the flexible control of components and concentrations in HEAs SNRs for achieving a library of HEA SNRs and also superior electrocatalytic properties. The well-designed HEA SNRs show great improvement in catalyzing the oxygen reduction reaction of fuel cells and also high discharge capacity, low charge overpotential, and excellent durability for Li-O2 batteries. DFT calculations reveal the superior electrochemical performances are attributed to the strong reduction capability from high-concentration reductive elements in HEAs, while the other elements guarantee the site-to-site efficient electron transfer.

18.
Adv Mater ; 34(30): e2202943, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35613477

RESUMEN

Medium-entropy alloy aerogels (MEAAs) with the advantages of both multimetallic alloys and aerogels are promising new materials in catalytic applications. However, limited by the immiscible behavior of different metals, achieving single-phase MEAAs is still a grand challenge. Herein, a general strategy for preparing ultralight 3D porous MEAAs with the lowest density of 39.3 mg cm-3 among the metal materials is reported, through combining auto-combustion and subsequent low-temperature reduction procedures. The homogenous mixing of precursors at the ionic level makes the short-range diffusion of metal atoms possible to drive the formation of single-phase MEAAs. As a proof of concept in catalysis, as-synthesized Ni50 Co15 Fe30 Cu5 MEAAs exhibit a high mass activity of 1.62 A mg-1 and specific activity of 132.24 mA cm-2 toward methanol oxidation reactions, much higher than those of the low-entropy counterparts. In situ Fourier transform infrared and NMR spectroscopies reveal that MEAAs can enable highly selective conversion of methanol to formate. Most importantly, a methanol-oxidation-assisted MEAAs-based water electrolyzer can achieve a low cell voltage of 1.476 V at 10 mA cm-2 for making value-added formate at the anode and H2 at the cathode, 173 mV lower than that of traditional alkaline water electrolyzers.

19.
J Colloid Interface Sci ; 605: 667-673, 2022 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-34364006

RESUMEN

Although the electrochemical production of hydrogen has been considered as a promising strategy to obtain the sustainable resources, the sluggish kinetics of anodic oxygen evolution reaction (OER) hindered the sustainable energy development. Herein, we design mesoporous cobalt ferrite phosphides hybridized on reduced graphene oxide (rGO) as a highly efficient bifunctional catalyst through a simple nanocasting method. The hybrid catalyst possesses the abundant interface, which provides the large active sites, as well as the hybrid rGO accelerates the electron exchange and ion diffusion. Moreover, the mesoporous structure not only prevents the aggregation of actives sites, but also benefits for the rapid escape of bubbles during catalytical process, which can significantly improve the catalytic performance. Consequently, the resulting mCo0.5Fe0.5P/rGO shows superior catalytic performance with a low overpotential of 250 mV at a current density of 10 mA cm-2 for OER and outstanding long-term stability. More importantly, an electrolyzer with mCo0.5Fe0.5P/rGO as both anode and cathode catalysts shows a low voltage of 1.66 V to afford a current density of 10 mA cm-2. This work offers a new route for designing the highly efficient OER and overall water splitting electrocatalysts.

20.
Small Methods ; 5(6): e2100154, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-34927914

RESUMEN

Ultrathin nanosheet catalysts deliver great potential in catalyzing the oxygen reduction reaction (ORR), but encounter the ceiling of the surface atomic utilizations, thus presenting a challenge associated with further boosting catalytic activity. Herein, a kind of PdPtCu ultrathin nanorings with increased numbers of electrocatalytically active sites is reported, with the purpose of breaking the activity ceiling of conventional catalysts. The as-made PdPtCu nanorings possess abundant high-index facets at the edge of both the exterior and interior surfaces. An ultrahigh electrochemical active surface area of 92.2 m2 g-1 PGM is achieved on this novel catalyst, much higher than that of the commercial Pt/C catalyst. The optimized Pd39 Pt33 Cu28 /C shows a great enhanced ORR activity with a specific activity of 2.39 mA cm-2 and a mass activity of 1.97 A mg-1 PGM at 0.9 V (versus RHE), as well as superior durability within 30 000 cycles. Density function theory calculations reveal that the high-index facets and alloying Cu atoms can optimize the oxygen adsorption energy, explaining the enhanced ORR activity. Overcoming a key technical barrier in sub-nanometer electrocatalysts, this work successfully introduces the hollow structures into the ultrathin nanosheets, heralding the exciting prospects of high-performance ORR catalysts in fuel cells.

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