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1.
Nat Commun ; 13(1): 4600, 2022 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-35933410

RESUMO

High-performance and low-cost photocatalysts play the key role in achieving the large-scale solar hydrogen production. In this work, we report a liquid-exfoliation approach to prepare NiPS3 ultrathin nanosheets as a versatile platform to greatly improve the light-induced hydrogen production on various photocatalysts, including TiO2, CdS, In2ZnS4 and C3N4. The superb visible-light-induced hydrogen production rate (13,600 µmol h-1 g-1) is achieved on NiPS3/CdS hetero-junction with the highest improvement factor (~1,667%) compared with that of pure CdS. This significantly better performance is attributed to the strongly correlated NiPS3/CdS interface assuring efficient electron-hole dissociation/transport, as well as abundant atomic-level edge P/S sites and activated basal S sites on NiPS3 ultrathin nanosheets advancing hydrogen evolution. These findings are revealed by the state-of-art characterizations and theoretical computations. Our work for the first time demonstrates the great potential of metal phosphorous chalcogenide as a general platform to tremendously raise the performance of different photocatalysts.

2.
Nanomaterials (Basel) ; 12(9)2022 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-35564273

RESUMO

Nitrogen (N) doping is an effective strategy for improving the solar-driven photocatalytic performance of anatase TiO2, but controllable methods for nitrogen-rich doping and associated defect engineering are highly desired. In this work, N-rich doped anatase TiO2 nanoparticles (4.2 at%) were successfully prepared via high-temperature nitridation based on thermally stable H3PO4-modified TiO2. Subsequently, the associated deep-energy-level defects such as oxygen vacancies and Ti3+ were successfully healed by smart photo-Fenton oxidation treatment. Under visible-light irradiation, the healed N-doped TiO2 exhibited a ~2-times higher activity of gas-phase acetaldehyde degradation than the non-treated one and even better than standard P25 TiO2 under UV-visible-light irradiation. The exceptional performance is attributed to the extended spectral response range from N-rich doping, the enhanced charge separation from hole capturing by N-doped species, and the healed defect levels with the proper thermodynamic ability for facilitating O2 reduction, depending on the results of ∙O2- radicals and defect measurement by electron spin resonance, X-ray photoelectron spectroscopy, atmosphere-controlled surface photovoltage spectra, etc. This work provides an easy and efficient strategy for the preparation of high-performance solar-driven TiO2 photocatalysts.

3.
Nanoscale ; 14(22): 8041-8049, 2022 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-35622376

RESUMO

Developing efficient Z-scheme heterojunctions with wide visible-light responsive perylene diimide (PDI) is highly desired for CO2 conversion, while the effective charge transfer and separation are crucial. Herein, TiO2-modulated tetra(4-carboxyphenyl)porphyrin/perylene diimide (T-TP/PDI) organic nano-heterojunctions have been fabricated for CO2 reduction, in which TP and PDI are first assembled via π-π interactions between their similar 2D conjugate structures, and then the TiO2 nanoparticles (ca. 10 nm) are anchored as an energy platform through the carboxyl groups on TP. The optimal one exhibits a ∼10-fold enhancement in photocatalytic activity compared with the pristine PDI. Based on the time-resolved surface photovoltage responses, electron paramagnetic resonance signals, in situ diffuse reflectance infrared Fourier transform spectra and the amount evaluation of H2O2 as the water-oxidation intermediate, it is suggested that the exceptional photoactivity be ascribed to the accelerated charge transfer and separation resulting from the constructed Z-scheme nano-heterojunctions with intimate interfacial interactions and the introduced energy platform TiO2 oriented towards largely inhibiting the type-II charge transfer pathway. This work diversifies the strategies for constructing efficient organic Z-scheme heterojunctions, and provides insight into interface correlation among components.

4.
J Hazard Mater ; 425: 127990, 2022 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-34986565

RESUMO

The development of highly-sensitive fluorescence detection systems for environmental contaminants has become high priority research in the past years. Special attention has been paid to graphitic carbon nitride (g-C3N4)-based nanomaterials, whose unique and superior optical property makes them promising and attractive candidates for this purpose. It is necessary to enhance the current understanding of the various classes of g-C3N4-based fluorescence detection systems and their mechanisms, as well as find suitable approaches to improve detection performance for environmental monitoring, protection, and management. In this review, the recent progresses on g-C3N4-based fluorescence detections for environmental contaminants, mainly including their basic principles, mechanisms, applications, modification strategies, and conclusions, are summarized. A particular emphasis is placed on the design and development of modification strategies for g-C3N4 with the objective of improving detection performance. High photoluminescence quantum yield, tunable fluorescence emission characteristics, and strong adsorption capacity of g-C3N4 could ensure the ultrasensitivity and selectivity of fluorescence detection of environmental contaminants. Concluding perspectives on the challenges and opportunities to design highly efficient g-C3N4-based fluorescence detection system are intensively put forward as well.


Assuntos
Nanoestruturas , Fluorescência
5.
J Colloid Interface Sci ; 608(Pt 3): 2921-2931, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-34799045

RESUMO

The exploitation of efficient electrocatalyst is significantly important for degradation of refractory organic pollutants. Herein, a novel Ti/CoTiO3/Ce-PbO2 composite electrocatalyst (abbreviated as CTO/CP) is successfully constructed via facile consecutive immersion pyrolysis and electro-deposition method and then systematically characterized by scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Fourier Transform infrared spectroscopy (FT-IR), energy dispersive spectroscopy (EDS) and near infrared chemical imaging (NIR-CI). Importantly, the electrochemical measurements demonstrate that the CTO/CP possesses numerous prominent properties such as lower charge transfer resistance, larger electroactive area, higher oxygen evolution potential than those of the pristine Ti/CoTiO3 (CTO) and Ti/Ce-PbO2 (CP). Thereby, the CTO/CP exhibits an enhanced electrocatalytic degradation performance with the degradation efficiency as high as 90.0% and COD removal rate of 88.3% at 180 min for the optimal CTO/CP (denoted as 10 layers of CTO and 1 h electrodeposition of CP), in which the ·OH is the major reactive species. Additionally, the optimal CTO/CP also shows a higher ICE/ACE together with lower EEC and desirable stability, universal applicability for many different dyes and reusability. Overall, this work offers a promising approach for enhancing the electrocatalytic properties of CTO via introducing CP.


Assuntos
Corantes , Poluentes Químicos da Água , Eletrodos , Oxirredução , Óxidos , Espectroscopia de Infravermelho com Transformada de Fourier , Titânio , Poluentes Químicos da Água/análise
6.
Adv Mater ; 33(48): e2105482, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34569106

RESUMO

The configuration regulation of single-atom photocatalysts (SAPCs) can significantly influence the interfacial charge transfer and subsequent catalytic process. The construction of conventional SAPCs for aqueous CO2 reduction is mainly devoted toward favorable activation and photoreduction of CO2 , however, the role of water is frequently neglected. In this work, single Ni atoms are successfully anchored by boron-oxo species on g-C3 N4 nanosheets through a facile ion-exchange method. The dative interaction between the B atom and the sp2 N atom of g-C3 N4 guarantees the high dispersion of boron-oxo species, where O atoms coordinate with single Ni (II) sites to obtain a unique six-oxygen-coordinated configuration. The optimized single-atom Ni photocatalyst, rivaling Pt-modified g-C3 N4 nanosheets, provides excellent CO2 reduction rate with CO and CH4 as products. Quasi-in-situ X-ray photoelectron spectra, transient absorption spectra, isotopic labeling, and in situ Fourier transform infrared spectra reveal that as-fabricated six-oxygen-coordinated single Ni (II) sites can effectively capture the photoelectrons of CN along the BO bridges and preferentially activate adsorbed water to produce H atoms to eventually induce a hydrogen-assisted CO2 reduction. This work diversifies the synthetic strategies for single-atom catalysts and provides insight on correlation between the single-atom configuration and reaction pathway.

7.
Small ; 17(32): e2100296, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34270858

RESUMO

Owing to dwindling fossil fuels reserves, the development of alternative renewable energy sources is globally important. Photocatalytic hydrogen (H2 ) evolution represents a practical and affordable alternative to convert sunlight into carbon-free H2 fuel. Recently, 2D/2D van der Waals heterostructures (vdWHs) have attracted significant research attention for photocatalysis. Here, for the first time a ReS2 /In2 ZnS4 2D/2D vdWH synthesized via a facile physical mixing is reported. It exhibits a highly promoted photocatalytic H2 -evolution rate of 2515 µmol h-1 g-1 . Importantly, this exceeds that for pristine In2 ZnS4 by about 22.66 times. This, therefore, makes ReS2 /In2 ZnS4 one of the most efficient In2 ZnS4 -based photocatalysts without noble-metal cocatalysts. Advanced characterizations and theoretical computations results show that interlayer electronic interaction within ReS2 /In2 ZnS4 vdWH and atomic-level S active centers along the edges of ReS2 NSs work collaboratively to result in the boosted light-induced H2 evolution. Results will be of immediate benefit in the rational design and preparation of vdWHs for applications in catalysis/(opto)electronics.

8.
Angew Chem Int Ed Engl ; 60(38): 20906-20914, 2021 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-34255409

RESUMO

A universal strategy is developed to construct a cascade Z-Scheme system, in which an effective energy platform is the core to direct charge transfer and separation, blocking the unexpected type-II charge transfer pathway. The dimension-matched (001)TiO2 -g-C3 N4 /BiVO4 nanosheet heterojunction (T-CN/BVNS) is the first such model. The optimized cascade Z-Scheme exhibits ≈19-fold photoactivity improvement for CO2 reduction to CO in the absence of cocatalysts and costly sacrificial agents under visible-light irradiation, compared with BVNS, which is also superior to other reported Z-Scheme systems even with noble metals as mediators. The experimental results and DFT calculations based on van der Waals structural models on the ultrafast timescale reveal that the introduced T as the platform prolongs the lifetimes of spatially separated electrons and holes and does not compromise their reduction and oxidation potentials.

9.
Bioresour Technol ; 326: 124794, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33550210

RESUMO

For solving the challenge in nitrate removal from low C/N wastewater at low temperature, Pseudomonas sp. Y39-6 was isolated and used in nitrate removal. It showed aerobic-heterotrophic denitrification with rate of 1.77 ± 0.31 mg/L·h and unusual aerobic-autotrophic nitrate removal (rate of 0.324 mg/L·h). The aerobic-autotrophic nitrate removal mechanisms were deep investigated by analyzing the nitrate removal process and genomic information. At aerobic-autotrophic condition, the strain Y39-6 could assimilate nitrate to amino acid (NO3- + PHA + CO2 â†’ C5H7O2N) with the carbon source from Polyhydroxyalkanoic acid (PHA) degradation and CO2 fixation. Flagella motivation, swarming activity and extracellular polymeric substances (EPS) production regulated Pseudomonas sp. Y39-6 forming biofilm. Carriers immobilized with Pseudomonas sp. Y39-6 were used in moving bed biofilm reactor (MBBR) and achieved 24.83% nitrate removal at C/N < 1 and 4 °C. Results of this study provided a practical way for nitrogen removal from low C/N wastewater in cold region.


Assuntos
Nitratos , Águas Residuárias , Biofilmes , Reatores Biológicos , Desnitrificação , Nitrogênio , Pseudomonas , Temperatura
10.
Adv Sci (Weinh) ; 7(16): 2001543, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32832373

RESUMO

Realization of solar-driven aerobic organic transformation under atmospheric pressure raises the great challenge for efficiently activating O2 by tailored photocatalysts. Guided by theoretical calculation, phosphate groups are used to induce the construction of ultrathin Co phthalocyanine/g-C3N4 heterojunctions (CoPc/P-CN, ≈4 nm) via strengthened H-bonding interfacial connection, achieving an unprecedented 14-time photoactivity improvement for UV-vis aerobic 2,4-dichlorophenol degradation compared to bulk CN by promoted activation of O2. It is validated that more •O2 - radicals are produced through the improved photoreduction of O2 by accelerated photoelectron transfer from CN to the ligand of CoPc and then to the abundant single Co-N4 (II) catalytic sites, as endowed by the matched dimension, intimate interface even at the molecular level, and high CoPc dispersion of resulted heterojunctions. Interestingly, CoPc/P-CN also exhibits outstanding photoactivities in the aerobic oxidation of aromatic alcohols. This work showcases a feasible route to realize efficient photocatalytic O2 activation by exploiting the potential of ultrathin metal phthalocyanine (MPc) assemblies with abundant single-atom sites. More importantly, a universal facile strategy of H-bonding-dominating construction of MPc-involved heterojunctions is successfully established.

11.
ACS Appl Mater Interfaces ; 12(25): 28264-28272, 2020 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-32490657

RESUMO

It is a great challenge for achieving efficiently controllable conversion of chlorinated organics through BiVO4-based photoelectrochemical methods by improving the selective adsorption of such organics and charge separation. Herein, we have successfully fabricated SnO2/010 facet-exposed BiVO4 nanocomposites by a series of hydrothermal processes and further used as efficient photoanodes. The resulting photoanode exhibits about 6.3 times higher photoelectrochemical activity than bulk-BiVO4, especially with the efficiently controllable conversion of 2,4-dichlorophenol (2,4-DCP) to the nontoxic valuable intermediates such as catechol and pyrogallol by preferential dechlorination. Based on the 2,4-DCP adsorption curves, in situ diffuse reflectance infrared spectra, transient-state surface photovoltage responses, and photocurrent action spectra, it was clearly confirmed that the exceptional performance could be mainly attributed to the promoted selective adsorption of 2,4-DCP for efficiently modulating holes by the strong coordination interactions between -Cl with lone-pair electrons in 2,4-DCP and Bi- with empty orbits on (010) facet-exposed BiVO4 nanoflakes and to the coupled nano-SnO2 for prolonging the charge lifetime of BiVO4 by acting as the high-energy-level electron-accepting platform. This work provides a feasible strategy to develop excellent BiVO4-based photoelectrochemical methods for efficiently controlling the conversion of chlorinated organics simultaneously with energy production and recovery.

12.
Inorg Chem ; 59(12): 8369-8379, 2020 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-32468810

RESUMO

With the reported CO2 activation for the oxidation of benzene to phenol (-ENE → -OL) by the graphitic carbon nitride g-C3N4 (CN) via an artificial photosynthetic route as inspiration, high-valent actinyls (AnmO2)n+ (An = U, Np, Pu; m = VI, V; n = 2, 1) have been introduced for its further modification. Our calculations indicate thermodynamic spontaneity in the feasibility of g-C3N4-(AnmO2)n+ (CN-Anm) formation. The magnificent structural and electronic properties of CN-Anm are utilized for CO2 activation in terms of the rarely studied -ENE → -OL conversion. The calculated free energies show that most steps of the catalytic cycle are favored by CN-Anm complexes. The first step (carbamate formation) is slightly endothermic in all cases, where CN-U is 0.51 eV higher than CN and CN-Pu is -0.01 eV lower. All benzene addition reactions release energy, with that for CN-U being the lowest. The phenolate formation is favored by some actinyl complexes over CN, and CN-U is only 0.23 eV higher. The phenol release (resulting in formamide complexes) and CO desorption are exothermic for all CN-Anm. The overall process suggests the improved catalytic performance of actinyl-modified CN materials, and the slightly depleted uranyl-carbon nitride could be one of the promising catalysts.

13.
Nanoscale ; 12(18): 10010-10018, 2020 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-32350498

RESUMO

It is highly desirable to improve charge separation and to provide catalytic functions for the efficient photocatalytic CO2 reduction reaction (CO2RR) on g-C3N4 (CN). Here, dimension-matched ultrathin NiMOF/CN heterojunctions have been successfully constructed by the in situ growth of NiMOF nanosheets on hydroxylated and 1,4-aminobenzoic acid (AA) functionalized CN nanosheets, respectively, with ultrasonic assistance. The resultant NiMOF/CN heterojunctions exhibited excellent photocatalytic activities for the CO2RR to produce CO and CH4, especially NiMOF/CN-AA, which had photoactivity 18 times higher than that of bare CN. Based on the surface photovoltage responses, wavelength-dependent photocurrent action spectra, electrochemical impedance spectra, and CO2 electrochemical reduction data, it is clearly confirmed that the exceptional photoactivity mainly resulted from the favorable charge transport properties of ultrathin CN and coupled NiMOF, and from the greatly enhanced charge separation via excited high-level electron transfer from CN to NiMOF in the resultant intimately contacted heterojunction caused by the induction effect of AA, and also from the provided catalytic functionality of the central Ni(ii) for CO2 activation. This work provides a feasible synthetic protocol to fabricate MOF-containing dimension-matched heterojunctions with good charge separation for efficient photocatalysis.

14.
Chem Commun (Camb) ; 56(36): 4926-4929, 2020 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-32239036

RESUMO

Ultrathin zinc phthalocyanine/graphene/BiVO4 heterojunctions have been successfully synthesized for efficient wide visible-light catalytic conversion of CO2 to CO with 14-time photoactivity improvement compared to the bare BiVO4 nanosheet, attributed to the strengthened Z-scheme charge transfer and separation by increasing the optimized amount of highly dispersed ZnPc via the pre-modified graphene-modulated assembly.

15.
ChemSusChem ; 13(14): 3707-3717, 2020 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-32134177

RESUMO

It is highly desired to improve the visible-light activity of g-C3 N4 for H2 evolution by constructing closely contacted heterojunctions with conductive polymers. Herein, a polymer nanocomposite photocatalyst with high visible-light activity is fabricated successfully by coupling nanosized polypyrrole (NPPy) particles onto g-C3 N4 nanosheets through a simple wet-chemical process, and its visible-light activity is improved further by constructing Mg-O bridges between the NPPy and g-C3 N4 . The amount-optimized bridged nanocomposite displays an approximately ninefold improvement in visible-light activity compared with g-C3 N4 . On the basis of transient-state surface photovoltage responses, photoluminescence spectra, . OH amount evaluation, and photoelectrochemical curves, it is concluded that the exceptional photoactivity can be attributed to the significantly promoted charge transfer and separation along with visible photosensitization from NPPy. Interestingly, it is confirmed that the promoted charge separation depends mainly on the excited high-level electron transfer from g-C3 N4 to NPPy by single-wavelength photocurrent action spectra. This work provides a feasible strategy for designing polymer nano-heterojunction photocatalysts with exceptional visible-light activities.

16.
Chem Commun (Camb) ; 56(2): 197-200, 2019 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-31750461

RESUMO

A triple sequential junction by rationally combining anatase/rutile nanoparticle TiO2 heterophase (Ans/R) and rutile/rutile TiO2 homophase (Rns/R) junctions was fabricated as a proof of concept. Such a continuous charge separation and transfer channel resulted in a remarkable enhancement in the separation of photogenerated carriers and the photocatalytic activity.

17.
Adv Sci (Weinh) ; 6(22): 1902170, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31763158

RESUMO

To achieve substantial reductions in CO2 emissions, catalysts for the photoreduction of CO2 into value-added chemicals and fuels will most likely be at the heart of key renewable-energy technologies. Despite tremendous efforts, developing highly active and selective CO2 reduction photocatalysts remains a great challenge. Herein, a metal oxide heterostructure engineering strategy that enables the gas-phase, photocatalytic, heterogeneous hydrogenation of CO2 to CO with high performance metrics (i.e., the conversion rate of CO2 to CO reached as high as 1400 µmol g cat-1 h-1) is reported. The catalyst is comprised of indium oxide nanocrystals, In2O3- x (OH) y , nucleated and grown on the surface of niobium pentoxide (Nb2O5) nanorods. The heterostructure between In2O3- x (OH) y nanocrystals and the Nb2O5 nanorod support increases the concentration of oxygen vacancies and prolongs excited state (electron and hole) lifetimes. Together, these effects result in a dramatically improved photocatalytic performance compared to the isolated In2O3- x (OH) y material. The defect optimized heterostructure exhibits a 44-fold higher conversion rate than pristine In2O3- x (OH) y . It also exhibits selective conversion of CO2 to CO as well as long-term operational stability.

18.
Angew Chem Int Ed Engl ; 58(32): 10873-10878, 2019 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-31199043

RESUMO

Cascade charge transfer was realized by a H-bond linked zinc phthalocyanine/BiVO4 nanosheet (ZnPc/BVNS) composite, which subsequently works as an efficient wide-visible-light-driven photocatalyst for converting CO2 into CO and CH4 , as shown by product analysis and 13 C isotopic measurement. The optimized ZnPc/BVNS nanocomposite exhibits a ca. 16-fold enhancement in the quantum efficiency compared with the reported BiVO4 nanoparticles at the excitation of 520 nm with an assistance of 660 nm photons. Experimental and theoretical results show the exceptional activities are attributed to the rapid charge separation by a cascade Z-scheme charge transfer mechanism formed by the dimension-matched ultrathin (ca. 8 nm) heterojunction nanostructure. The central Zn2+ in ZnPc could accept the excited electrons from the ligand and then provide a catalytic function for CO2 reduction. This Z-scheme is also feasible for other MPc, such as FePc and CoPc, together with BVNS.

19.
Chemistry ; 25(41): 9670-9677, 2019 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-31069880

RESUMO

As photocatalysis technology could transform renewable and clean solar energy into green hydrogen (H2 ) energy through solar water splitting, it is regarded as the "Holy Grail" in chemistry field in the 21st century. Unfortunately, the bottleneck of this technique still lies in the exploration of highly active, cost-effective, and robust photocatalysts. This work reports the design and synthesis of a novel zeolitic imidazole framework (ZIF) coupled Zn0.8 Cd0.2 S hetero-structured photocatalyst for high-performance visible-light-induced H2 production. State-of-the-art characterizations and theoretical computations disclose that the interfacial electronic interaction between ZIF and Zn0.8 Cd0.2 S, the high distribution of Zn0.8 Cd0.2 S on ZIF, and the atomically dispersed coordinately unsaturated Co sites in ZIF synergistically arouse the significantly improved visible-light photocatalytic H2 production performance.

20.
Nanoscale ; 11(17): 8304-8309, 2019 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-30982842

RESUMO

The rapid consumption of non-renewable fossil fuels and the relevant critical environmental issues have significantly boosted the demand for clean, renewable and carbon-free energy sources. The conversion of solar energy into green hydrogen (H2) via photocatalytic water splitting stands out as a promising, cost-effective and environmentally friendly technology. However, the realization of large-scale solar-driven photocatalytic H2 production relies on the development of inexpensive, efficient and stable photocatalysts. Here, for the first time, we report the fabrication of Zn0.8Cd0.2S (ZCS) nanoparticles (NPs) dispersed Co-based metal-organic layers (CMLs) using an easy self-assembly approach. The as-synthesized ZCS/CML composite shows a remarkable visible-light-induced H2-production activity of 18 102 µmol h-1 g-1, 492% higher than that of pure ZCS. A series of advanced characterization studies, e.g., synchrotron-based X-ray absorption near edge structure and time-resolved photoluminescence spectroscopy, disclose that the strong electronic interaction between ZCS and CML and the abundant reactive sites on the CML lead to the significantly improved photocatalytic H2-production activity. Our contribution not only demonstrates the application of CML as an earth-abundant support and promoter to tremendously boost photocatalytic H2 production without noble-metal co-catalysts, but also sheds light on the tailored design and synthesis of metal-organic-layer based materials for energy conversion and storage.

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