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Showing papers by "Wuhan University of Technology published in 2021"


Journal ArticleDOI
TL;DR: Experimental results show that the AOA provides very promising results in solving challenging optimization problems compared with eleven other well-known optimization algorithms.

1,218 citations


Journal ArticleDOI
TL;DR: In this paper, a pyrene-based conjugated polymer is synthesized via the typical Suzuki-Miyaura reactions, and then employed as a substrate to anchor CdS nanocrystals.
Abstract: Inspired by natural photosynthesis, constructing inorganic/organic heterojunctions is regarded as an effective strategy to design high-efficiency photocatalysts. Herein, a step (S)-scheme heterojunction photocatalyst is prepared by in situ growth of an inorganic semiconductor firmly on an organic semiconductor. A new pyrene-based conjugated polymer, pyrene-alt-triphenylamine (PT), is synthesized via the typical Suzuki-Miyaura reactions, and then employed as a substrate to anchor CdS nanocrystals. The optimized CdS/PT composite, coupling 2 wt% PT with CdS, exhibits a robust H2 evolution rate of 9.28 mmol h-1 g-1 with continuous release of H2 bubbles, as well as a high apparent quantum efficiency of 24.3%, which is ≈8 times that of pure CdS. The S-scheme charge transfer mechanism between PT and CdS, is systematically demonstrated by photoirradiated Kelvin probe measurement and in situ irradiated X-ray photoelectron spectroscopy analyses. This work provides a protocol for preparing specific S-scheme heterojunction photocatalysts on the basis of inorganic/organic coupling.

369 citations


Journal ArticleDOI
TL;DR: In this article, a dual-metal atomically dispersed Fe,Mn/N-C catalyst was proposed for oxygen reduction reaction applied to fuel cells and metal-air batteries.
Abstract: As low-cost electrocatalysts for oxygen reduction reaction applied to fuel cells and metal-air batteries, atomic-dispersed transition metal-nitrogen-carbon materials are emerging, but the genuine mechanism thereof is still arguable. Herein, by rational design and synthesis of dual-metal atomically dispersed Fe,Mn/N-C catalyst as model object, we unravel that the O2 reduction preferentially takes place on FeIII in the FeN4 /C system with intermediate spin state which possesses one eg electron (t2g4eg1) readily penetrating the antibonding π-orbital of oxygen. Both magnetic measurements and theoretical calculation reveal that the adjacent atomically dispersed Mn-N moieties can effectively activate the FeIII sites by both spin-state transition and electronic modulation, rendering the excellent ORR performances of Fe,Mn/N-C in both alkaline and acidic media (halfwave positionals are 0.928 V in 0.1 M KOH, and 0.804 V in 0.1 M HClO4), and good durability, which outperforms and has almost the same activity of commercial Pt/C, respectively. In addition, it presents a superior power density of 160.8 mW cm−2 and long-term durability in reversible zinc–air batteries. The work brings new insight into the oxygen reduction reaction process on the metal-nitrogen-carbon active sites, undoubtedly leading the exploration towards high effective low-cost non-precious catalysts. The working mechanism of several low-cost electrocatalyst materials is still arguable. Here the authors show a model Fe,Mn/N-C catalyst where the oxygen reduction preferentially takes place on Fe(III) sites with the intermediate spin state (t2g4 eg1) caused by the adjacent Mn-N moieties.

327 citations


Journal ArticleDOI
01 Oct 2021-Small
TL;DR: In this paper, a step-scheme core-shell TiO2 @ZnIn2 S4 heterojunction was designed for photocatalytic CO2 reduction. But the performance of the optimized sample was limited by the large specific surface areas and abundant active sites.
Abstract: Reasonable design of efficient hierarchical photocatalysts has gained significant attention. Herein, a step-scheme (S-scheme) core-shell TiO2 @ZnIn2 S4 heterojunction is designed for photocatalytic CO2 reduction. The optimized sample exhibits much higher CO2 photoreduction conversion rates (the sum yield of CO, CH3 OH, and CH4 ) than the blank control, i.e., ZnIn2 S4 and TiO2 . The improved photocatalytic performance can be attributed to the inhibited recombination of photogenerated charge carriers induced by S-scheme heterojunction. The improvement is also attributed to the large specific surface areas and abundant active sites. Meanwhile, S-scheme photogenerated charge transfer mechanism is testified by in situ irradiated X-ray photoelectron spectroscopy, work function calculation, and electron paramagnetic resonance measurements. This work provides an effective strategy for designing highly efficient heterojunction photocatalysts for conversion of solar fuels.

291 citations


Journal ArticleDOI
TL;DR: In this article, a series of sulfur-doped g-C3N4 (SCN)/TiO2 S-scheme photocatalysts were synthesized using electrospinning and calcination methods.

281 citations



Journal ArticleDOI
TL;DR: Xiaolei et al. as discussed by the authors presented a Memory-efficient, Visualization-enhanced, and Parallel-accelerated R package called "rMVP" to address the need for improved GWAS computation.

260 citations


Journal ArticleDOI
TL;DR: In this paper, a review of the safety properties of SIBs is presented and several effective materials design concepts are also discussed, which can be used to improve the battery safety.
Abstract: DOI: 10.1002/aenm.202000974 and the relatively high cell cost raises concerns on the sustainable development of LIBs, especially in the large-scale energy storage area, which put specific requirements on the price cost, safety, and durability of the battery.[1] In addition to the concern over potential shortage of lithium, the incidents associated with fires and explosions of state-of-the-art LIBs are stimulating advanced strategies and new safe alternatives in recent years. Sodium-ion batteries (SIBs), with identical internal components and working principles with LIBs, have been proposed as one of the most promising nextgeneration energy storage technology because of the evident advantages of lowcost and worldwide abundance of charge carriers.[2] Besides, the cost of SIBs could be further reduced by use of Co/Ni-free cathode materials[3] and aluminum current collector on the anode side since sodium does not alloy with aluminum.[4] In addition to the economic benefits, the configuration of SIBs offers a potentially safe way for batteries storage and transportation. Since Al current collector does not dissolve into electrolyte at a voltage of 0 V, shipping and storing SIBs which contain no energy (a fully discharged state) is potentially feasible.[5] Moreover, Dahn’s group investigated the thermal stability of positive materials for SIBs and found that the desodiated Na0.5CrO2 cathode was less reactive than Li0FePO4 in nonaqueous electrolyte at elevated temperatures.[6] Robinson et al. found that the self-heating rate in a Na-ion pouch cell is significantly slower than that in a commercial LiCoO2 (LCO) pouch cell and the thermal runaway process is less exothermic for Na-ion cells, indicating that SIBs could be a potentially safer option compared with LIBs.[7] However, the larger and heavier Na ions have poor kinetic characteristic in the host structure during insertion reaction process, so it may lead to rapid degradation of the host materials with exothermic reaction.[8–10] In addition, the higher solubility of solid electrolyte interphase (SEI) of SIBs resulting from lower Lewis acidity of sodium complex, indicates that the incomplete coverage of electrode may further lead to undesired side reactions, accelerating heat generation. The cathode materials reported so far, roughly including oxides, polyanions, organics, Prussian blue and its analogues, which have poor electronic/ionic conductivity, will bring issues to thermal diffusion as well.[11] So far, nonaqueous liquid electrolyte is still the primary option for SIBs because of wide electrochemical stable window, high ionic conductivity, and rapid mass transfer at the electrolyteelectrode interface, yet giving rise to safety hazards.[12] Recent Sodium-ion batteries, with their evident superiority in resource abundance and cost, are emerging as promising next-generation energy storage systems for large-scale applications, such as smart grids and low-speed electric vehicles. Accidents related to fires and explosions for batteries are a reminder that safety is prerequisite for energy storage systems, especially when aiming for grid-scale use. In a typical electrochemical secondary battery, the electrical power is stored and released via processes that generate thermal energy, leading to temperature increments in the battery system, which is the main cause for battery thermal abuse. The investigation of the energy generated during the chemical/electrochemical reactions is of paramount importance for battery safety, unfortunately, it has not received the attention it deserves. In this review, the fundamentals of the heat generation, accumulation, and transportation in a battery system are summarized and recent key research on materials design to improve sodium-ion battery safety is highlighted. Several effective materials design concepts are also discussed. This review is designed to arouse the attention of researcher and scholars and inspire further improvements in battery safety.

252 citations


Journal ArticleDOI
TL;DR: In this article, a series of polydopamine-modified TiO2 hollow spheres were fabricated by in situ self-polymerization of dopamine to systematically investigate the effect of PDA wrapping on the photocatalytic CO2 reduction activities.
Abstract: Photocatalytic CO2 conversion into solar fuels has been a promising strategy to utilize abundant solar energy and alleviate greenhouse effect. Herein, a series of polydopamine-modified TiO2 (TiO2@PDA) hollow spheres were fabricated by in situ self-polymerization of dopamine to systematically investigate the effect of PDA wrapping on the photocatalytic CO2 reduction activities of TiO2. Among all TiO2@PDA composite photocatalysts, the highest value of methane yield (1.50 μmol h−1 g−1) was achieved with 0.5 % PDA, which was 5 times than that of pure TiO2 (0.30 μmol h−1 g−1). The improvement of photocatalytic activity and methane selectivity was ascribed to the enhanced light absorption, promoted CO2 adsorption capacity, increased reduction power of photogenerated electrons, as well as efficient separation and transfer of photogenerated charge carriers induced by the S-scheme heterojunction between TiO2 and PDA. This work provides a facile surface modification method with cost-effective polymer materials in photocatalytic CO2 conversion.

243 citations


Journal ArticleDOI
18 Jun 2021-Science
TL;DR: In this article, a lead halide-templated crystallization strategy is developed for printing formamidinium (FA)-cesium (Cs) lead triiodide perovskite films.
Abstract: Upscaling efficient and stable perovskite layers is one of the most challenging issues in the commercialization of perovskite solar cells. Here, a lead halide-templated crystallization strategy is developed for printing formamidinium (FA)-cesium (Cs) lead triiodide perovskite films. High-quality large-area films are achieved through controlled nucleation and growth of a lead halide•N-methyl-2-pyrrolidone adduct that can react in situ with embedded FAI/CsI to directly form α-phase perovskite, sidestepping the phase transformation from δ-phase. A nonencapsulated device with 23% efficiency and excellent long-term thermal stability (at 85°C) in ambient air (~80% efficiency retention after 500 hours) is achieved with further addition of potassium hexafluorophosphate. The slot die-printed minimodules achieve champion efficiencies of 20.42% (certified efficiency 19.3%) and 19.54% with an active area of 17.1 and 65.0 square centimeters, respectively.

241 citations


Journal ArticleDOI
TL;DR: In this article, a review of nitrogen-doped graphene (NG) is presented, which summarizes in situ and ex situ synthesis methods, highlights the mechanism and advantages of NG in photocatalysis, and outlines its applications in different photocATalysis directions (primarily hydrogen production, CO2 reduction, pollutant degradation and as photoactive ingredient).
Abstract: Solving energy and environmental problems through solar-driven photocatalysis is an attractive and challenging topic. Hence, various types of photocatalysts have been developed successively to address the demands of photocatalysis. Graphene-based materials have elicited considerable attention since the discovery of graphene. As a derivative of graphene, nitrogen-doped graphene (NG) particularly stands out. Nitrogen atoms can break the undifferentiated structure of graphene and open the bandgap while endowing graphene with an uneven electron density distribution. Therefore, NG retains nearly all the advantages of original graphene and is equipped with several novel properties, ensuring infinite possibilities for NG-based photocatalysis. This review introduces the atomic and band structures of NG, summarizes in situ and ex situ synthesis methods, highlights the mechanism and advantages of NG in photocatalysis, and outlines its applications in different photocatalysis directions (primarily hydrogen production, CO2 reduction, pollutant degradation, and as photoactive ingredient). Lastly, the central challenges and possible improvements of NG-based photocatalysis in the future are presented. This study is expected to learn from the past and achieve progress toward the future for NG-based photocatalysis.

Journal ArticleDOI
TL;DR: In this paper, hierarchical ZnMn2O4/ZnO nanofibers were prepared as photocatalysts by electrospinning and calcination, and the results showed that the charge separation efficiency in the composite was significantly elevated.

Journal ArticleDOI
16 Jun 2021-Joule
TL;DR: In this paper, a ternary all-polymer solar cells (TPSC) with a near-infrared acceptor PY2F-T and paired with polymer donor PM6 was designed to achieve a power conversion efficiency of 17.2%.

Journal ArticleDOI
TL;DR: Li et al. as mentioned in this paper designed the shell-thickness-controlled Ni3C@Ni/g-C3N4 photocatalysts with intimate Schottky-junctions by an in situ high-temperature transformation strategy.
Abstract: Herein, we designed the shell-thickness-controlled Ni3C@Ni/g-C3N4 photocatalysts with intimate Schottky-junctions by an in situ high-temperature transformation strategy. Meanwhile, we found that the cocatalysts with optimized Ni shell-layer thickness of 15 nm could achieve the best visible-light photocatalytic H2-production performance of 11.28 μmolh−1, with an apparent quantum yield (AQY) of 1.49 % at 420 nm, which was 16 times higher than that of Ni3C/g-C3N4. Moreover, an excellent stability is achieved. The well-defined density functional theory (DFT) calculations indicate that the “TOP_C1” sites of Ni3C@Ni can exhibit the H adsorption and Gibbs free energies of -0.07eV and 0.18 eV, respectively, which should be hydrogen-evolution active sites instead of two “HOLLOW” sites. Interestingly, the intimate Schottky-junctions, could hinder rapid charge recombination, increase reactive sites, boost catalytic kinetics and passivate unstable surface of Ni3C, thus achieving shell-thickness-dependent hydrogen evolution. Therefore, the Ni3C@Ni core–shell cocatalysts will open a new avenue for robust solar fuel production.

Journal ArticleDOI
TL;DR: In this paper, the electronic metal-support interaction (EMSI) plays a crucial role in catalysis as it can induce electron transfer between metal and support, modulate the electronic state of the supported metal, and optimize the reduction of intermediate species.
Abstract: The electronic metal-support interaction (EMSI) plays a crucial role in catalysis as it can induce electron transfer between metal and support, modulate the electronic state of the supported metal, and optimize the reduction of intermediate species In this work, the tailoring of electronic structure of Pt single atoms supported on N-doped mesoporous hollow carbon spheres (Pt1 /NMHCS) via strong EMSI engineering is reported The Pt1 /NMHCS composite is much more active and stable than the nanoparticle (PtNP ) counterpart and commercial 20 wt% Pt/C for catalyzing the electrocatalytic hydrogen evolution reaction (HER), exhibiting a low overpotential of 40 mV at a current density of 10 mA cm-2 , a high mass activity of 207 A mg-1 Pt at 50 mV overpotential, a large turnover frequency of 2018 s-1 at 300 mV overpotential, and outstanding durability in acidic electrolyte Detailed spectroscopic characterizations and theoretical simulations reveal that the strong EMSI effect in a unique N1 -Pt1 -C2 coordination structure significantly tailors the electronic structure of Pt 5d states, resulting in promoted reduction of adsorbed proton, facilitated H-H coupling, and thus Pt-like HER activity This work provides a constructive route for precisely designing single-Pt-atom-based robust electrocatalysts with high HER activity and durability

Journal ArticleDOI
TL;DR: In this paper, the removal of heavy metals and dyes by clay-based adsorbents, from natural clays to 1D clay nanotubes and 2D Clay nanosheets, has been summarized.

Journal ArticleDOI
08 Jul 2021-Science
TL;DR: In this article, the authors developed SnSe crystals with a wide bandgap of 33 kBT with attractive thermoelectric properties through Pb alloying, which achieved an ultra-high power factor of 75 μWcm-1K-2 at 300 K and a ZTave of 1.90.
Abstract: Thermoelectric materials transfer heat and electrical energy, being useful for power generation or cooling applications. Many of these materials have narrow bandgaps, especially for cooling applications where this property has been seen as particularly important for enhancing the thermoelectric properties. We developed SnSe crystals with a wide bandgap Eg ~ 33 kBT with attractive thermoelectric properties through Pb alloying. The momentum and energy multiband alignment promoted by Pb alloying resulted in an ultra-high power factor ~75 μWcm–1K–2 at 300 K, and a ZTave ~ 1.90. We show that a 31-pair thermoelectric device can produce a power generation efficiency ~4.4% and a cooling ΔTmax ~ 45.7 K. These results demonstrate that wide bandgap compounds can be used for thermoelectric cooling applications.

Journal ArticleDOI
TL;DR: In this article, a model-driven scheme with dual stages is proposed to compensate the dynamic pressure measurement, which is applied to an industrial hydraulic pipe system, and the experimental results show that the relative error is reduced greatly after the compensation is implemented, demonstrating the validity of the proposed method.
Abstract: Strain-based non-intrusive approaches for measuring the pressure of pipes have attracted widespread attention due to their great convenience and ability to avoid destroying the integrity of structures. However, the mentioned method usually measures the dynamic pressure based only on the static strain–pressure sensitivity coefficients (SSSCs) instead of the dynamic strain–pressure sensitivity coefficients (DSSCs) due to its complicated calibration, which will inevitably affect the accuracy significantly. To address this issue, a model-driven scheme with dual stages is proposed in the present study to compensate the dynamic pressure measurement. The DSSCs are analytically derived for the first time from the axial governing equations of the pipe, considering the general boundary conditions for the thin-walled and thick-walled pipes simultaneously. In the first stage, the physical parameters involved in the DSSCs are calibrated by minimizing the residual of the experimental results and the theoretical counterparts. In the second stage, the DSSCs calculated from the calibrated analytical model are utilized to compensate the dynamic pressure based on the relationship between the DSSCs and the SSSCs. The proposed method is applied to an industrial hydraulic pipe system, and the experimental results show that the relative error is reduced greatly after the compensation is implemented, demonstrating the validity of the proposed compensation method.

Journal ArticleDOI
TL;DR: In this article, the role of water molecules in rechargeable aqueous Zn-ion batteries (AZIBs) has been discussed from the perspective of the electrolyte, Zn anode, and cathode materials.
Abstract: Benefiting from loose assembly conditions, a high level of safety and environmentally friendly characteristics, rechargeable aqueous Zn-ion batteries (AZIBs) have attracted significant attention. The electrochemical kinetics and performance of the AZIBs are greatly affected by water in electrolytes or electrode materials. The corrosion and passivation of the Zn electrode caused by the inevitable solvation process of water molecules can lead to the growth of dendrites, thus resulting in a limited cycle life. Moreover, water in the electrode material, whether in the form of structural water or co-intercalated hydrated cations, can greatly affect the electrochemical behavior due to its small size, high polarity and hydrogen bonding. Unlike previous reports, this review focuses on the roles of water molecules during electrochemical processes in AZIBs. We comprehensively summarize the influencing mechanisms of water molecules during the energy storage process from the perspectives of the electrolyte, Zn anode, and cathode materials, and further include the basic theory, modification methods, and practical applications. The mystery concerning the water molecules and the electrochemical performance of AZIBs is revealed herein, and we also propose novel insights and actionable methods regarding the potential future directions in the design of high-performance AZIBs.

Journal ArticleDOI
Hongxia Huang1, Ting Guo1, Kai Wang1, Yuan Li1, Gaoke Zhang1 
TL;DR: The electron spin resonance (ESR) analysis indicated that the generation of the sulfate radicals, hydroxyl radicals, and superoxide radicals was greatly promoted in the MRSB/PS system, which might give a new way to reuse abandoned rape straw and synthesize new recyclable catalysts for activating PS to degrade organic pollutants in water.

Journal ArticleDOI
TL;DR: In this article, a comprehensive review of the environmental and energy applications of 2D MXenes is presented, including organic pollutant degradation, water splitting for H2 evolution, CO2 reduction, nitrogen fixation, H2O2 production, antibacterial application, desulfurization and denitrogenation of fuels.

Journal ArticleDOI
TL;DR: In this paper, a facile design of a phosphorus/imidazole-containing single-component epoxy (EP) resins via incorporating 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10oxide (DOPO) and a flame-retardant curing agent cyclotriphosphazene-modified BICP (BICP) into EP is presented.
Abstract: The design of highly fire-safe and smoke-suppressive single-component epoxy (EP) resins combining modest curing temperature and fast curing rate has been desirable yet very challenging in both academia and industry. Herein, we report a facile design of a phosphorus/imidazole-containing single-component EP system via incorporating 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) and a flame-retardant curing agent cyclotriphosphazene-modified benzimidazole (BICP) into EP. Our results show that EP/DOPO/BICP exhibits a rapid modest-temperature curing feature because DOPO serves as a switch that triggers BICP to release benzimidazole (BIM) via substitution reaction in the initial curing stage. Moreover, as-prepared EP/DOPO/BICP shows outstanding fire retardancy, reflected by the high limited oxygen index (LOI) of 38.3% and UL-94 V-0 rating. Compared to the control EP system, the peak of heat release rate (PHRR) and total smoke production (TSP) of EP/DOPO/BICP remarkably decrease by ~74.5% and ~50.6%, respectively, which is superior to previously-reported flame-retardant P-containing epoxy counterparts. The significant enhancements in flame retardancy and smoke suppression are mainly due to the formation of a highly intumescent char layer and the reduced burning degree of pyrolysis fragments. This work offers a facile and scalable strategy for creating fast-curing, modest-temperature curable, highly fire-resistant and smoke-suppressive one-component epoxy systems applicable to large-scale industrial production.

Journal ArticleDOI
TL;DR: In this article, the authors proposed an attention mechanism-based convolutional neural network-long short-term memory (AMCNN-LSTM) model to accurately detect anomalies.
Abstract: Since edge device failures (i.e., anomalies) seriously affect the production of industrial products in Industrial IoT (IIoT), accurately and timely detecting anomalies are becoming increasingly important. Furthermore, data collected by the edge device contain massive user’s private data, which is challenging current detection approaches as user privacy has attracted more and more public concerns. With this focus, this article proposes a new communication-efficient on-device federated learning (FL)-based deep anomaly detection framework for sensing time-series data in IIoT. Specifically, we first introduce an FL framework to enable decentralized edge devices to collaboratively train an anomaly detection model, which can improve its generalization ability. Second, we propose an attention mechanism-based convolutional neural network-long short-term memory (AMCNN-LSTM) model to accurately detect anomalies. The AMCNN-LSTM model uses attention mechanism-based convolutional neural network units to capture important fine-grained features, thereby preventing memory loss and gradient dispersion problems. Furthermore, this model retains the advantages of the long short-term memory unit in predicting time-series data. Third, to adapt the proposed framework to the timeliness of industrial anomaly detection, we propose a gradient compression mechanism based on Top- ${k}$ selection to improve communication efficiency. Extensive experimental studies on four real-world data sets demonstrate that our framework accurately and timely detects anomalies and also reduces the communication overhead by 50% compared to the FL framework that does not use the gradient compression scheme.

Journal ArticleDOI
TL;DR: In this paper, a hybrid catalyst CdS/Ag2S/NiS is synthesized via hydrothermal and photodeposition methods, which shows a drastically elevated hydrogen production rate of 48.3 mmol g−1 h−1 under visible light.
Abstract: Cocatalysts play an indispensable role in photocatalytic H2 production via water splitting for the conversion of solar energy into storable chemical energy. Herein, the hybrid catalyst CdS/Ag2S/NiS is synthesized via hydrothermal and photodeposition methods. CdS/Ag2S/NiS shows a drastically elevated hydrogen production rate of 48.3 mmol g−1 h−1 under visible light due to the combined merits of the Schottky junction between CdS and metal-like Ag2S and the constructed p–n junction between CdS and NiS. Time-resolved photoluminescence spectroscopy and photochemical tests reveal the accelerated charge transfer and significantly reduced electron–hole pair recombination. Further investigation with in-situ surface photovoltage imaging technology demonstrates that the reduction cocatalyst Ag2S and oxidation cocatalyst NiS can serve as photogenerated electron and hole traps, respectively. This research not only provides insight into designing high-efficiency photocatalyst for hydrogen production but also utilize a brand new method for the confirmation of charge–carrier migration pathways.

Journal ArticleDOI
TL;DR: Fe/Zn-SBC had the high selective adsorption capacity for TC and CIP in a wide pH range and even at the high ionic strength, and suggested that it is a promising adsorbent for antibiotics removal.

Journal ArticleDOI
TL;DR: This review systematically summarizes several important advances in complete reconstruction for the first time, which includes fundamental understandings of complete reconstruction, the characteristics and advantages of completely reconstructed catalysts, and their design principles.
Abstract: Reconstruction induced by external environment (such as applied voltage bias and test electrolytes) changes catalyst component and catalytic behaviors. Investigations of complete reconstruction in energy conversion recently receive intensive attention, which promote the targeted design of top-performance materials with maximum component utilization and good stability. However, the advantages of complete reconstruction, its design strategies, and extensive applications have not achieved the profound understandings and summaries it deserves. Here, this review systematically summarizes several important advances in complete reconstruction for the first time, which includes 1) fundamental understandings of complete reconstruction, the characteristics and advantages of completely reconstructed catalysts, and their design principles, 2) types of reconstruction-involved precatalysts for oxygen evolution reaction catalysis in wide pH solution, and origins of limited reconstruction degree as well as design strategies/principles toward complete reconstruction, 3) complete reconstruction for novel material synthesis and other electrocatalysis fields, and 4) advanced in situ/operando or multiangle/level characterization techniques to capture the dynamic reconstruction processes and real catalytic contributors. Finally, the existing major challenges and unexplored/unsolved issues on studying the reconstruction chemistry are summarized, and an outlook for the further development of complete reconstruction is briefly proposed. This review will arouse the attention on complete reconstruction materials and their applications in diverse fields.

Journal ArticleDOI
TL;DR: Theoretical calculations elucidate that the introduction of axial oxygen atom could optimize surface states of Ni-N4 moieties and enhance the charge polarization effect, therefore decreasing the potential barrier of intermediate COOH* formation, a key factor to accelerate the reaction kinetics and boost the CO2RR performance.
Abstract: Regulating the local environment and structure of metal center coordinated by nitrogen ligands (M-N4 ) to accelerate overall reaction dynamics of the electrochemical CO2 reduction reaction (CO2 RR) has attracted extensive attention. Herein, we develop an axial traction strategy to optimize the electronic structure of the M-N4 moiety and construct atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom, which are embedded within the carbon matrix (Ni-N4 -O/C). The Ni-N4 -O/C electrocatalyst exhibited excellent CO2 RR performance with a maximum CO Faradic efficiency (FE) close to 100 % at -0.9 V. The CO FE could be maintained above 90 % in a wide range of potential window from -0.5 to -1.1 V. The superior CO2 RR activity is due to the Ni-N4 -O active moiety composed of a Ni-N4 site with an additional oxygen atom that induces an axial traction effect.

Journal ArticleDOI
TL;DR: A poly(vinylidene fluoride-co-hexafluoropropylene)-based polymer-in-salt solid electrolyte (PISSE) with high room-temperature ionic conductivity presents high performance close to that with liquid electrolyte, which also exhibits robust flexibility and brilliant safety under abuse tests.
Abstract: Solid-state lithium batteries (SSLBs) are promising owing to enhanced safety and high energy density but plagued by the relatively low ionic conductivity of solid-state electrolytes and large electrolyte-electrode interfacial resistance. Herein, we design a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based polymer-in-salt solid electrolyte (PISSE) with high room-temperature ionic conductivity (1.24×10-4 S cm-1 ) and construct a model integrated TiO2 /Li SSLB with 3D fully infiltration of solid electrolyte. With forming aggregated ion clusters, unique ionic channels are generated in the PISSE, providing much faster Li+ transport than common polymer electrolytes. The integrated device achieves maximized interfacial contact and electrochemical and mechanical stability, with performance close to liquid electrolyte. A pouch cell made of 2 SSLB units in series shows high voltage plateau (3.7 V) and volumetric energy density comparable to many commercial thin-film batteries.

Journal ArticleDOI
TL;DR: CAC-5 (modified AC) exhibits better CO2 adsorption performance, which can be attributed to the formation of the CO2-philic active sites on AC surface by N-species, and the high IAST selectivity factor for N-doped ACs indicates their excellent Adsorption selectivity for CO2 over N2.

Journal ArticleDOI
TL;DR: In this article, a large-area LSC (100 × 225 cm2) based on colloidal carbon quantum dots (C-dots) synthesized via a space-confined vacuum-heating approach was presented.
Abstract: Luminescent solar concentrators (LSCs) are large-area sunlight collectors coupled to small area solar cells, for efficient solar-to-electricity conversion. The three key points for the successful market penetration of LSCs are: (i) removal of light losses due to reabsorption during light collection; (ii) high light-to-electrical power conversion efficiency of the final device; (iii) long-term stability of the LSC structure related to the stability of both the matrix and the luminophores. Among various types of fluorophores, carbon quantum dots (C-dots) offer a wide absorption spectrum, high quantum yield, non-toxicity, environmental friendliness, low-cost, and eco-friendly synthetic methods. However, they are characterized by a relatively small Stokes shift, compared to inorganic quantum dots, which limits the highest external optical efficiency that can be obtained for a large-area single-layer LSC (>100 cm2) based on C-dots below 2%. Herein, we report highly efficient large-area LSCs (100–225 cm2) based on colloidal C-dots synthesized via a space-confined vacuum-heating approach. This one batch reaction could produce Gram-scale C-dots with a high quantum yield (QY) (∼65%) using eco-friendly citric acid and urea as precursors. Thanks to their very narrow size distribution, the C-dots produced via the space-confined vacuum-heating approach had a large Stokes shift of 0.53 eV, 50% larger than C-dots synthesized via a standard solvothermal reaction using the same precursors with a similar absorption range. The large-area LSC (15 × 15 × 0.5 cm3) prepared by using polyvinyl pyrrolidone (PVP) polymer as a matrix exhibited an external optical efficiency of 2.2% (under natural sun irradiation, 60 mW cm−2, uncharacterized spectrum). After coupling to silicon solar cells, the LSC exhibited a power conversion efficiency (PCE) of 1.13% under natural sunlight illumination (20 mW cm−2, uncharacterized spectrum). These unprecedented results were obtained by completely suppressing the reabsorption losses during light collection, as proved by optical spectroscopy. These findings demonstrate the possibility of obtaining eco-friendly, high-efficiency, large-area LSCs through scalable production techniques, paving the way to the lab-to-fab transition of this kind of devices.