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1.
Nat Commun ; 15(1): 3753, 2024 May 04.
Article in English | MEDLINE | ID: mdl-38704394

ABSTRACT

The European ammonia industry emits 36 million tons of carbon dioxide annually, primarily from steam methane reforming (SMR) hydrogen production. These emissions can be mitigated by producing hydrogen via water electrolysis using dedicated renewables with grid backup. This study investigates the impact of decarbonization targets for hydrogen synthesis on the economic viability and technical feasibility of retrofitting existing European ammonia plants for on-site, semi-islanded electrolytic hydrogen production. Results show that electrolytic hydrogen cuts emissions, on average, by 85% (36%-100% based on grid price and carbon intensity), even without enforcing emission limits. However, an optimal lifespan average well-to-gate emission cap of 1 kg carbon dioxide equivalent (CO2e)/kg H2 leads to a 95% reduction (92%-100%) while maintaining cost-competitiveness with SMR in renewable-rich regions (mean levelized cost of hydrogen (LCOH) of 4.1 euro/kg H2). Conversely, a 100% emissions reduction target dramatically increases costs (mean LCOH: 6.3 euro/kg H2) and land area for renewables installations, likely hindering the transition to electrolytic hydrogen in regions with poor renewables and limited land. Increasing plant flexibility effectively reduces costs, particularly in off-grid plants (mean reduction: 32%). This work guides policymakers in defining cost-effective decarbonization targets and identifying region-based strategies to support an electrolytic hydrogen-fed ammonia industry.

2.
Nat Commun ; 15(1): 2617, 2024 Mar 23.
Article in English | MEDLINE | ID: mdl-38521862

ABSTRACT

Recent advancements in membrane-assisted seawater electrolysis powered by renewable energy offer a sustainable path to green hydrogen production. However, its large-scale implementation faces challenges due to slow power-to-hydrogen (P2H) conversion rates. Here we report a modular forward osmosis-water splitting (FOWS) system that integrates a thin-film composite FO membrane for water extraction with alkaline water electrolysis (AWE), denoted as FOWSAWE. This system generates high-purity hydrogen directly from wastewater at a rate of 448 Nm3 day-1 m-2 of membrane area, over 14 times faster than the state-of-the-art practice, with specific energy consumption as low as 3.96 kWh Nm-3. The rapid hydrogen production rate results from the utilisation of 1 M potassium hydroxide as a draw solution to extract water from wastewater, and as the electrolyte of AWE to split water and produce hydrogen. The current system enables this through the use of a potassium hydroxide-tolerant and hydrophilic FO membrane. The established water-hydrogen balance model can be applied to design modular FO and AWE units to meet demands at various scales, from households to cities, and from different water sources. The FOWSAWE system is a sustainable and an economical approach for producing hydrogen at a record-high rate directly from wastewater, marking a significant leap in P2H practice.

3.
Eur J Ophthalmol ; : 11206721241235266, 2024 Feb 23.
Article in English | MEDLINE | ID: mdl-38396370

ABSTRACT

OBJECTIVES: to evaluate long-term effectiveness and safety of fluocinolone acetonide (FAc) implant used as second-line treatment in patients with persistent diabetic macular edema (DME). METHODS: retrospective data chart review of 241 pseudophakic eyes of 178 patients treated with FAc from July 2017 to December 2021 in 10 medical retinal units in Italy. The primary endpoint was the change of best-corrected visual acuity (BCVA) and central macular thickness (CMT) at 2 years. A Student's paired t-test was used. Additional therapies for DME and intraocular pressure (IOP)-related events were also evaluated. RESULTS: efficacy of FAc was assessed in a subset of 111 eyes with at least 24 months of follow-up. Mean BCVA increased at 2 years by 5.1 ETDRS letters (95%CI = 2.6-7.5; p < 0.001) while mean CMT decreased by 189 µm (95% CI 151-227; p < 0.001). Thirty-eight of these eyes (34.2%) needed additional intravitreal treatments, mainly anti-VEGF. Safety was evaluated on the entire cohort of 241 eyes treated with FAc. Overall, 66 eyes (27.4%) required emergent IOP-lowering medications (typically within the first-year post FAc) while 14 eyes (5.8%) underwent trabeculectomy, mostly during the second year of follow-up. CONCLUSION: FAc implant provides a substantial long-term functional and anatomical benefit when used as second-line treatment in eyes with DME. IOP rise can be adequately managed with topical agents although some eyes may require IOP-lowering surgery.

4.
Nat Commun ; 14(1): 7984, 2023 Dec 02.
Article in English | MEDLINE | ID: mdl-38042884

ABSTRACT

Protonic ceramic fuel cells with high efficiency and low emissions exhibit high potential as next-generation sustainable energy systems. However, the practical proton conductivity of protonic ceramic electrolytes is still not satisfied due to poor membrane sintering. Here, we show that the dynamic displacement of Y3+ adversely affects the high-temperature membrane sintering of the benchmark protonic electrolyte BaZr0.1Ce0.7Y0.1Yb0.1O3-δ, reducing its conductivity and stability. By introducing a molten salt approach, pre-doping of Y3+ into A-site is realized at reduced synthesis temperature, thus suppressing its further displacement during high-temperature sintering, consequently enhancing the membrane densification and improving the conductivity and stability. The anode-supported single cell exhibits a power density of 663 mW cm-2 at 600 °C and long-term stability for over 2000 h with negligible performance degradation. This study sheds light on protonic membrane sintering while offering an alternative strategy for protonic ceramic fuel cells development.

5.
Small ; 19(39): e2302691, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37279776

ABSTRACT

Composite polymer-ceramic electrolytes have shown considerable potential for high-energy-density Li-metal batteries as they combine the benefits of both polymers and ceramics. However, low ionic conductivity and poor contact with electrodes limit their practical usage. In this study, a highly conductive and stable composite electrolyte with a high ceramic loading is developed for high-energy-density Li-metal batteries. The electrolyte, produced through in situ polymerization and composed of a polymer called poly-1,3-dioxolane in a poly(vinylidene fluoride)/ceramic matrix, exhibits excellent room-temperature ionic conductivity of 1.2 mS cm-1 and high stability with Li metal over 1500 h. When tested in a Li|electrolyte|LiFePO4 battery, the electrolyte delivers excellent cycling performance and rate capability at room temperature, with a discharge capacity of 137 mAh g-1 over 500 cycles at 1 C. Furthermore, the electrolyte not only exhibits a high Li+ transference number of 0.76 but also significantly lowers contact resistance (from 157.8 to 2.1 Ω) relative to electrodes. When used in a battery with a high-voltage LiNi0.8 Mn0.1 Co0.1 O2 cathode, a discharge capacity of 140 mAh g-1 is achieved. These results show the potential of composite polymer-ceramic electrolytes in room-temperature solid-state Li-metal batteries and provide a strategy for designing highly conductive polymer-in-ceramic electrolytes with electrode-compatible interfaces.

6.
J Phys Chem Lett ; 14(20): 4688-4695, 2023 May 25.
Article in English | MEDLINE | ID: mdl-37171053

ABSTRACT

Replacing fossil fuels with renewable energy sources is a crucial step for mitigating global warming. However, the intermittent nature of the most prevalent renewable sources, such as solar and wind, poses a significant challenge to their widespread deployment. One potential solution for renewable sources of storage is power-to-X, which involves the production of chemicals from electricity using solid oxide electrolysis cells. This process offers a flexible and efficient means of energy storage. This Perspective offers an overview of the characteristics, capabilities, and fundamental mechanisms of solid oxide electrolysis cells. It also examines the latest research progress and explores the prospects and challenges in this field.

7.
Small Methods ; 7(7): e2201714, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37029582

ABSTRACT

The sluggish kinetics of the oxygen reduction reaction (ORR) with complex multielectron transfer steps significantly limits the large-scale application of electrochemical energy devices, including metal-air batteries and fuel cells. Recent years witnessed the development of metal oxide-supported metal catalysts (MOSMCs), covering single atoms, clusters, and nanoparticles. As alternatives to conventional carbon-dispersed metal catalysts, MOSMCs are gaining increasing interest due to their unique electronic configuration and potentially high corrosion resistance. By engineering the metal oxide substrate, supported metal, and their interactions, MOSMCs can be facilely modulated. Significant progress has been made in advancing MOSMCs for ORR, and their further development warrants advanced characterization methods to better understand MOSMCs and precise modulation strategies to boost their functionalities. In this regard, a comprehensive review of MOSMCs for ORR is still lacking despite this fast-developing field. To eliminate this gap, advanced characterization methods are introduced for clarifying MOSMCs experimentally and theoretically, discuss critical methods of boosting their intrinsic activities and number of active sites, and systematically overview the status of MOSMCs based on different metal oxide substrates for ORR. By conveying methods, research status, critical challenges, and perspectives, this review will rationally promote the design of MOSMCs for electrochemical energy devices.

8.
Small Methods ; 7(4): e2201138, 2023 Apr.
Article in English | MEDLINE | ID: mdl-36843320

ABSTRACT

Perovskites have shown tremendous promise as functional materials for several energy conversion and storage technologies, including rechargeable batteries, (electro)catalysts, fuel cells, and solar cells. Due to their excellent operational stability and performance, high-entropy perovskites (HEPs) have emerged as a new type of perovskite framework. Herein, this work reviews the recent progress in the development of HEPs, including synthesis methods and applications. Effective strategies for the design of HEPs through atomistic computations are also surveyed. Finally, an outlook of this field provides guidance for the development of new and improved HEPs.

9.
Small ; 18(47): e2204109, 2022 Nov.
Article in English | MEDLINE | ID: mdl-36228095

ABSTRACT

Perovskite oxides are intriguing electrocatalysts for the oxygen evolution reaction, but both surface (e.g., composition) and bulk (e.g., lattice oxygen) properties should be optimized to maximize their participation in offering favorable activity and durability. In this work, it is demonstrated that through introducing exogenous Fe3+ ( Fe exo 3 + ${\rm{Fe}}_{{\rm{exo}}}^{3 + }$ ) into the liquid electrolyte, not only is the reconstructed surface stabilized and optimized, but the lattice oxygen diffusion is also accelerated. As a result, compared to that in Fe-free 0.1 m KOH, PrBa0.5 Sr0.5 Co2 O5+δ in 0.1 m KOH + 0.1 mm Fe3+ demonstrates a tenfold increment in activity, an extremely low Tafel slope of ≈50 mV dec-1 , and outstanding stability at 10.0 mA cm-2  for 10 h. The superior activity and stability are further demonstrated in Zn-air batteries by presenting high open-circuit voltage, narrow potential gap, high power output, and long-term cycle stability (500 cycles). Based on experimental and theoretical calculations, it is discovered that the dynamical interaction between the Co hydr(oxy)oxide from surface reconstruction and intentional Fe3+ from the electrolyte plays an important role in the enhanced activity and durability, while the generation of a perovskite-hydr(oxy)oxide heterostructure improves the lattice oxygen diffusion to facilitate lattice oxygen participation and enhances the stability.

10.
Adv Sci (Weinh) ; 9(34): e2204800, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36266984

ABSTRACT

Urea oxidation reaction (UOR) with a low equilibrium potential offers a promising route to replace the oxygen evolution reaction for energy-saving hydrogen generation. However, the overpotential of the UOR is still high due to the complicated 6e- transfer process and adsorption/desorption of intermediate products. Herein, utilizing a cation exchange strategy, Ni-doped CuO nanoarrays grown on 3D Cu foam are synthesized. Notably, Ni-CuO NAs/CF requires a low potential of 1.366 V versus a reversible hydrogen electrode to drive a current density of 100 mA cm-2 , outperforming various benchmark electrocatalysts and maintaining robust stability in alkaline media. Theoretical and experimental studies reveal that Ni as the driving force center can effectively enhance the urea adsorption and stabilize CO*/NH* intermediates toward the UOR. These findings suggest a new direction for constructing nanostructures and modulating electronic structures, ultimately developing promising Cu-based electrode catalysts.

11.
Angew Chem Int Ed Engl ; 61(33): e202204990, 2022 Aug 15.
Article in English | MEDLINE | ID: mdl-35638132

ABSTRACT

Dry reforming of methane (DRM) has been emerging as a viable solution to achieving carbon neutrality enhanced by the Paris Agreement as it converts the greenhouse gases of CO2 and CH4 into industrially useful syngas. However, there have been limited studies on the DRM catalyst under mild operating conditions with a high dilution gas ratio due to their deactivation from carbon coking and metal sintering. Herein, we apply the triple-phase boundary (TPB) concept to DRM catalyst via exsolution phenomenon that can secure elongated TPB by controlling the Fe-doping ratio in perovskite oxide. Remarkably, the exsolved catalyst with prolongated TPB shows exceptional CO2 and CH4 conversion rates of 95.9 % and 91.6 %, respectively, stable for 1000 hours under a dilution-free system. DFT calculations confirm that the Lewis acid of support and Lewis base of metal at the TPB promote the adsorption of reactants, resulting in lowering the overall CO2 dissociation and CH4 dehydrogenation energy.

12.
Graefes Arch Clin Exp Ophthalmol ; 260(10): 3185-3195, 2022 Oct.
Article in English | MEDLINE | ID: mdl-35511286

ABSTRACT

PURPOSE: PERSEUS-IT (NCT02289924) was a prospective, observational, 2-year study evaluating the effectiveness and treatment patterns of intravitreal aflibercept (IVT-AFL) in patients with neovascular age-related macular degeneration (nAMD) in routine clinical practice in Italy. METHODS: Treatment-naïve patients with nAMD receiving IVT-AFL per routine clinical practice were enrolled. The primary endpoint was mean change in visual acuity (VA; decimals) from baseline to month (M) 12 and M24. Outcomes were evaluated for the overall study population and independently for the 2 treatment cohorts: regular (3 initial monthly doses, ≥ 7 injections by M12, and ≥ 4 injections between M12 and M24) and irregular (any other pattern). RESULTS: Of 813 patients enrolled, 709 were included in the full analysis set (FAS); VA assessments were available for 342 patients at M12 (FAS1Y, 140 regular and 202 irregular) and 233 patients at M24 (FAS2Y, 37 regular and 196 irregular). In the overall FAS, the mean ± SD change in VA from baseline to M12 and M24 was + 0.09 ± 0.24 and + 0.02 ± 0.25 decimals, and there was a statistically significant difference between the regular and irregular cohorts in both FAS1Y (p = 0.0034) and FAS2Y (p = 0.0222). Ocular treatment-emergent adverse events were reported in 4.1% (n = 33/810 [safety set]) of patients. CONCLUSION: In PERSEUS-IT, clinically relevant functional and anatomic improvements were observed within the first 12 months of IVT-AFL treatment in routine clinical practice in Italy in patients with treatment-naïve nAMD. These gains were generally maintained across the 2-year study. The safety profile of IVT-AFL was consistent with prior studies. TRIAL REGISTRATION NUMBER: ClinicalTrials.gov Identifier: NCT02289924. DATE OF REGISTRATION: November 13, 2014.


Subject(s)
Angiogenesis Inhibitors , Macular Degeneration , Humans , Intravitreal Injections , Macular Degeneration/drug therapy , Prospective Studies , Ranibizumab , Receptors, Vascular Endothelial Growth Factor/therapeutic use , Recombinant Fusion Proteins/therapeutic use , Treatment Outcome
13.
J Colloid Interface Sci ; 621: 222-231, 2022 Sep.
Article in English | MEDLINE | ID: mdl-35461137

ABSTRACT

Liquid organic electrolytes commonly employed in commercial Li-ion batteries suffer from safety issues such as flammability and explosions. Replacing liquid electrolytes with nonflammable electrolytes has become increasingly attractive in the development of safe, high-energy Li-metal batteries (LMBs). In this work, nonflammable, robust, and flexible composite polymer-polymer electrolytes (PPEs) were successfully fabricated by flame-retardant solution casting with polyimide (PI) and polyvinylidene fluoride (PVDF). The optimized nonflammable PPEs (e.g., PPE-50) demonstrate not only good mechanical properties (i.e., a high tensile strength of 29.6 MPa with an elongation at break of 87.2%), but also high Li salts dissolubility, the former of which ensures the suppression of Li dendrites, while the latter further improves the ionic conductivity (∼1.86 × 10-4 S cm-1 at 30 °C). The resulting symmetric cells (Li|PPE-50|Li) offer excellent Li stripping and plating stability for 1000 h at 0.5 mA cm-2/0.25 mAh cm-2 and 600 h at 2.0 mA cm-2/1.0 mAh cm-2. In addition, the LiFePO4|PPE-50|Li half cells show high cycling performance (e.g., a reversible discharge capacity of 135.9 mAh g-1 after 300 cycles at 1C) and rate capability (e.g., 117.2 mAh g-1 at 4C). The PPE-50 is also compatible with a high-voltage cathode (e.g., LiNi0.5Mn0.3Co0.2O2), and the resulting batteries demonstrate long-term cycling stability with a high cut-off voltage of 4.5 V vs. Li/Li+. Because of the incorporation of a mechanically robust and thermally stable PI, a polar PVDF, and flame-retardant trimethyl phosphate (TMP) within PPEs, as well as the coordination between Li salts and TMP, and the interaction between Li salts and polymers (especially between Li bis(oxalato)borate) and PI, as well as the bis(oxalato)borate anion and PI), PPEs show great potential for practical and high-energy LMBs without safety concerns.

14.
Small ; 18(16): e2200450, 2022 Apr.
Article in English | MEDLINE | ID: mdl-35277919

ABSTRACT

Anode-supported protonic ceramic fuel cells (PCFCs) are highly promising and efficient energy conversion systems. However, several challenges need to be overcome before these systems are used more widely, including the poor sintering of recently developed proton-conducting oxides and the decreased proton conductivity due to detrimental reactions between the nickel from anode and the electrolyte occurring during high-temperature co-sintering. Herein, a Ni doping strategy to increase the electrolyte sintering, suppress the detrimental phase reactions, and generate stable Ni nanoparticles for enhanced performance is proposed. A nickel-doped perovskite oxide is developed with the nominal composition of Ba(Zr0.1 Ce0.7 Y0.1 Yb0.1 )0.95 Ni0.05 O3- δ . Acting as a sintering aid, such a small amount of nickel effectively improves the sintering of the electrolyte. Concomitantly, reactions between nickel and the Ni-doped ceramic phase are suppressed, turning detrimental phase reactions into benefits. The nickel doping further promotes the formation of Ni nanoparticles, which enhance the electrocatalytic activity of the anode toward the hydrogen oxidation reaction and improve the charge transfer across the anode-electrolyte interface. As a result, highly efficient PCFCs are developed. The innovative anode developed in this work also shows favorable activity toward ammonia decomposition, making it highly promising for use in direct ammonia fuel cells.

15.
Small Methods ; 6(1): e2101017, 2022 Jan.
Article in English | MEDLINE | ID: mdl-35041274

ABSTRACT

Owing to the low theoretical potential of the urea oxidation reaction (UOR), urea electrolysis is an energy-saving technique for the generation of hydrogen. Herein, a hierarchical structure of CuO nanowires decorated with nickel hydroxide supported on 3D Cu foam is constructed. Combined theoretical and experimental analyses demonstrate the high reactivity and selectivity of CuO and Ni(OH)2 toward the UOR instead of the oxygen evolution reaction. The hierarchical structure creates a synergistic effect between the two highly active sites, enabling an exceptional UOR activity with a record low potential of 1.334 V (vs the reversible hydrogen electrode) to reach 100 mA cm-2 and a low Tafel slope of 14 mV dec-1 in 1 m KOH and 0.5 m urea electrolyte. Assembling full urea electrolysis driven by this developed UOR electrocatalyst as the anode and a commercial Pt/C electrocatalyst as the cathode provides a current density of 20 mA cm-2 at a cell voltage of ≈1.36 V with promising operational stability for at least 150 h. This work not only enriches the UOR material family but also significantly advances energy-saving hydrogen production.

16.
Eur J Ophthalmol ; 32(4): 2388-2394, 2022 Jul.
Article in English | MEDLINE | ID: mdl-34392710

ABSTRACT

PURPOSE: This is a retrospective, single-center, non randomized interventional real life study, investigating the correlation between variability of central retinal thickness (CRT) and functional outcomes during 2 years of anti-VEGF therapy in patients treated for neovascular age related macular degeneration (nAMD). BACKGROUND: CRT fluctuations can depend on various factors such as the correct timing of injections, the therapeutic algorithm, and the number of injections (NI) performed; it is important to understand if CRT fluctuations are responsible for worse visual outcomes and consequently to identify the correct ways to avoid or reduce them. METHODS: Forty-one patients were treated for nAMD with aflibercept: 0.5 mg intravitreal aflibercept was administered every 4 weeks during the first 3 months, then bimonthly over the first year, and after the first year adopting a PRN regimen. Standard deviation of CRT (CRT/SD), BCVA, and NI were recorded. Correlation studies were performed by Pearson's test, Ancova, and Principal Component Analysis. RESULTS: A negative correlation was found between CRT/SD and final BCVA. In patients who lost more than 15 letters, CRT/SD mean was significantly higher in comparison with patients who lost less than 15 letters. Patients with final BCVA >65 letters showed lower CRT/SD values compared to patients with final BCVA ⩽65 letters. Multivariate analysis confirmed that in patients with higher baseline BCVA, improvement of BCVA was correlated to NI, and lower values of CRT fluctuations were observed. CONCLUSIONS: CRT fluctuations, even after an appropriate NI given per year, significantly influence BCVA; a proactive treatment algorithm appears crucial when treating patients with nAMD.


Subject(s)
Angiogenesis Inhibitors , Macular Degeneration , Receptors, Vascular Endothelial Growth Factor , Angiogenesis Inhibitors/therapeutic use , Humans , Intravitreal Injections , Macular Degeneration/drug therapy , Receptors, Vascular Endothelial Growth Factor/therapeutic use , Recombinant Fusion Proteins/therapeutic use , Retrospective Studies , Treatment Outcome , Visual Acuity
17.
Small ; 17(45): e2104144, 2021 Nov.
Article in English | MEDLINE | ID: mdl-34605170

ABSTRACT

Perovskite-based oxides attract great attention as catalysts for energy and environmental devices. Nanostructure engineering is demonstrated as an effective approach for improving the catalytic activity of the materials. The mechanism for the enhancement, nevertheless, is still not fully understood. In this study, it is demonstrated that compressive strain can be introduced into freestanding perovskite cobaltite La0.8 Sr0.2 CoO3- δ (LSC) nanofibers with sufficient small size. Crystal structure analysis suggests that the LSC fiber is characterized by compressive strain along the ab plane and less distorted CoO6 octahedron compared to the bulk powder sample. Accompanied by such structural changes, the nanofiber shows significantly higher oxygen reduction reaction (ORR) activity and better stability at elevated temperature, which is attributed to the higher oxygen vacancy concentration and suppressed Sr segregation in the LSC nanofibers. First-principle calculations further suggest that the compressive strain in LSC nanofibers effectively shortens the distance between the Co 3d and O 2p band center and lowers the oxygen vacancy formation energy. The results clarify the critical role of surface stress in determining the intrinsic activity of perovskite oxide nanomaterials. The results of this work can help guide the design of highly active and durable perovskite catalysts via nanostructure engineering.

18.
Nat Commun ; 12(1): 5235, 2021 Sep 02.
Article in English | MEDLINE | ID: mdl-34475400

ABSTRACT

Single-atom catalysts have been widely investigated for several electrocatalytic reactions except electrochemical alcohol oxidation. Herein, we synthesize atomically dispersed platinum on ruthenium oxide (Pt1/RuO2) using a simple impregnation-adsorption method. We find that Pt1/RuO2 has good electrocatalytic activity towards methanol oxidation in an alkaline media with a mass activity that is 15.3-times higher than that of commercial Pt/C (6766 vs. 441 mA mg‒1Pt). In contrast, single atom Pt on carbon black is inert. Further, the mass activity of Pt1/RuO2 is superior to that of most Pt-based catalysts previously developed. Moreover, Pt1/RuO2 has a high tolerance towards CO poisoning, resulting in excellent catalytic stability. Ab initio simulations and experiments reveal that the presence of Pt‒O3f (3-fold coordinatively bonded O)‒Rucus (coordinatively unsaturated Ru) bonds with the undercoordinated bridging O in Pt1/RuO2 favors the electrochemical dehydrogenation of methanol with lower energy barriers and onset potential than those encountered for Pt‒C and Pt‒Ru.

19.
Materials (Basel) ; 14(11)2021 May 25.
Article in English | MEDLINE | ID: mdl-34070590

ABSTRACT

Our work proposes a comparison between Spark Plasma Sintering of LiFePO4 carried out using an Alternating Current (AC) and Direct Current (DC). It quantifies the Li-ion migration using DC, and it validates such hypothesis using impedance spectroscopy, X-ray photoelectron spectroscopy and inductively coupled plasma optical emission spectroscopy. The use of an AC field seems effective to inhibit undesired Li-ion migration and achieve high ionic conductivity as high as 4.5 × 10-3 S/cm, which exceeds by one order of magnitude samples processed under a DC field. These results anticipate the possibility of fabricating a high-performance all-solid-state Li-ion battery by preventing undesired Li loss during SPS processing.

20.
Adv Sci (Weinh) ; 8(15): e2002510, 2021 Aug.
Article in English | MEDLINE | ID: mdl-34155825

ABSTRACT

Hybrid organic-inorganic perovskites are one of the promising candidates for the next-generation semiconductors due to their superlative optoelectronic properties. However, one of the limiting factors for potential applications is their chemical and structural instability in different environments. Herein, the stability of (FAPbI3 )0.85 (MAPbBr3 )0.15 perovskite solar cell is explored in different atmospheres using impedance spectroscopy. An equivalent circuit model and distribution of relaxation times (DRTs) are used to effectively analyze impedance spectra. DRT is further analyzed via machine learning workflow based on the non-negative matrix factorization of reconstructed relaxation time spectra. This exploration provides the interplay of charge transport dynamics and recombination processes under environment stimuli and illumination. The results reveal that in the dark, oxygen atmosphere induces an increased hole concentration with less ionic character while ionic motion is dominant under ambient air. Under 1 Sun illumination, the environment-dependent impedance responses show a more striking effect compared with dark conditions. In this case, the increased transport resistance observed under oxygen atmosphere in equivalent circuit analysis arises due to interruption of photogenerated hole carriers. The results not only shed light on elucidating transport mechanisms of perovskite solar cells in different environments but also offer an effective interpretation of impedance responses.

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