Rhenium anchored Ti3C2T x (MXene) nanosheets for electrocatalytic hydrogen production.

Atomically thin Ti3C2T x (MXene) nanosheets with rich termination groups, acting as active sites for effective functionalization, are used as an efficient solid support to host rhenium (Re) nanoparticles for the electrocatalytic hydrogen evolution reaction (HER). The newly designed electrocatalyst - Re nanoparticles anchored on Ti3C2T x MXene nanosheets (Re@Ti3C2T x ) - exhibited promising catalytic activity with a low overpotential of 298 mV to achieve a current density of 10 mV cm-2, while displaying excellent stability. In comparison, the pristine Ti3C2T x MXene requires higher overpotential of 584 mV to obtain the same current density. After being stored under ambient conditions for 30 days, Re@Ti3C2T x retained 100% of its initial catalytic activity for the HER, while the pristine Ti3C2T x retained only 74.8% of its initial value. According to our theoretical calculations using density functional theory, dual Re anchored MXene (Re@Ti3C2T x ) exhibits a near-zero value of Gibbs free energy (ΔG H* = -0.06 eV) for the HER, demonstrating that the presence of Re significantly enhances the electrocatalytic activity of MXene nanosheets. This work introduces a facile strategy to develop an effective electrocatalyst for electrocatalytic hydrogen production.

Ultrastable Zinc Anode Enabled by CO2-Induced Interface Layer.

Aqueous Zn-ion batteries (AZIBs), being safe, inexpensive, and pollution-free, are a promising candidate for future large-scale sustainable energy storage. However, in a conventional AZIBs setup, the Zn metal anode suffers oxidative corrosion, side reactions with electrolytes, disordered dendrite growth during operation, and consequently low efficiency and short lifespan. In this work, we discover that purging CO2 gas into the electrolyte could address these issues by eliminating dissolved O2, inhibiting side reactions by buffering the local pH change, and preventing dendrite growth by inducing the in situ formation of a ZnCO3 solid electrolyte interphase layer. Moreover, the CO2-purged electrolyte could enable a highly reversible plating/stripping behavior with a high Coulombic efficiency of 99.97% and an ultralong lifespan of 32,000 cycles (1600 h) even under an ultrahigh current density of 40 mA cm-2. Consequently, the CO2-purged symmetrical cells deliver long cycling stability at a high depth of discharge of 57%, while the CO2-purged Zn/V2O5 full cells exhibit outstanding capacity retention of 66% after 1000 cycles at a high current density of 5 A g-1. Our strategy, the simple introduction of CO2 gas into the electrolyte, could effectively mediate the zinc anode's critical issues and provide a scalable and cost-effective pathway for the commercialization of AZIBs.

Cytomembrane-Inspired MXene Ink with Amphiphilic Surfactant for 3D Printed Microsupercapacitors.

Two-dimensional (2D) material-based hydrogels have been widely utilized as the ink for extrusion-based 3D printing in various electronics. However, the viscosity of the hydrogel ink is not high enough to maintain the self-supported structure without architectural deformation. It is also difficult to tune the microstructure of the printed devices using a low-viscosity hydrogel ink. Herein, by mimicking a phospholipid bilayer in a cytomembrane, the amphiphilic surfactant nonaethylene glycol monododecyl ether (C12E9) was incorporated into MXene hydrogel. The incorporation of C12E9 offers amphiphilicity to the MXene flakes and produces a 3D interlinked network of the MXene flakes. The 3D interlinked network offers a high-viscosity, homogenized flake distribution and enhanced printability to the ink. This ink facilitates the alignment of the MXene flakes during extrusion as well as the formation of the aligned micro- and sub-microsized porous structures, leading to the improved electrochemical performance of the printed microsupercapacitor. This study provides an example for the preparation of microelectronics with tunable microstructures.

Scalable Spray Drying Production of Amorphous V2 O5 -EGO 2D Heterostructured Xerogels for High-Rate and High-Capacity Aqueous Zinc Ion Batteries.

Rechargeable aqueous zinc-ion batteries (ZIBs) are promising in stationary grid energy storage due to their advantages in safety and cost-effectiveness, and the search for competent cathode materials is one core task in the development of ZIBs. Herein, the authors design a 2D heterostructure combining amorphous vanadium pentoxide and electrochemically produced graphene oxide (EGO) using a fast and scalable spray drying technique. The unique 2D heterostructured xerogel is achieved by controlling the concentration of EGO in the precursor solution. Driven by the improved electrochemical kinetics, the resultant xerogel can deliver an excellent rate capability (334 mAh g-1 at 5 A g-1 ) as well as a high specific capacity (462 mAh g-1 at 0.2 A g-1 ) as the cathode material in ZIB. It is also shown that the coin cell constructed based on spray-dried xerogel can output steady, high energy densities over a broad power density window. This work provides a scalable and cost-effective approach for making high performance electrode materials from cheap sources through existing industrialized materials processing.

Smart Solar-Metal-Air Batteries Based on BiOCl Photocorrosion for Monolithic Solar Energy Conversion and Storage.

Herein, a BiOCl hydrogel film electrode featuring excellent photocorrosion and regeneration properties acts as the anode to construct a novel type of smart solar-metal-air batteries (SMABs), which combines the characteristics of solar cells (direct photovoltaic conversion) and metal-air batteries (electric energy storage and release interacting with atmosphere). The cyclic photocorrosion processes between BiOCl (Bi3+ ) and Bi can simply be achieved by solar light illumination and standing in the dark. Upon illumination, the device takes open-circuit configuration to charge itself from the sunlight. Notably, in this system, the converted solar energy can be stored in the SMABs without the need of external assistance. In the discharging process in the dark, Bi0 spontaneously turns back to Bi3+ producing electrons to induce the oxygen reduction reaction. With an illumination of 15 min, the battery with an electrode area of 1 cm2 can be continuously discharged for ≈3000 s. Taking elemental Bi as the calculation object, the theoretical capacity of the SMABs is 384.75 mAh g-1 , showing its potential application in energy storage. This novel type of SMABs is developed based on the unique photocorrosive and self-oxidation reaction of BiOCl to achieve photochemical energy generation and storage.

Ambient Fabrication of Organic-Inorganic Hybrid Perovskite Solar Cells.

Organic-inorganic hybrid perovskite solar cells (PSCs) have attracted significant attention in recent years due to their high-power conversion efficiency, simple fabrication, and low material cost. However, due to their high sensitivity to moisture and oxygen, high efficiency PSCs are mainly constructed in an inert environment. This has led to significant concerns associated with the long-term stability and manufacturing costs, which are some of the major limitations for the commercialization of this cutting-edge technology. Over the past few years, excellent progress in fabricating PSCs in ambient conditions has been made. These advancements have drawn considerable research interest in the photovoltaic community and shown great promise for the successful commercialization of efficient and stable PSCs. In this review, after providing an overview to the influence of an ambient fabrication environment on perovskite films, recent advances in fabricating efficient and stable PSCs in ambient conditions are discussed. Along with discussing the underlying challenges and limitations, the most appropriate strategies to fabricate efficient PSCs under ambient conditions are summarized along with multiple roadmaps to assist in the future development of this technology.

Highly Dispersed Ru Nanoparticles on Boron-Doped Ti3 C2 Tx (MXene) Nanosheets for Synergistic Enhancement of Electrocatalytic Hydrogen Evolution.

2D-layered materials have attracted increasing attention as low-cost supports for developing active catalysts for the hydrogen evolution reaction (HER). In addition, atomically thin Ti3 C2 Tx (MXene) nanosheets have surface termination groups (Tx : F, O, and OH), which are active sites for effective functionalization. In this work, heteroatom (boron)-doped Ti3 C2 Tx (MXene) nanosheets are developed as an efficient solid support to host ultrasmall ruthenium (Ru) nanoparticles for electrocatalytic HER. The quantum-mechanical first-principles calculations and electrochemical tests reveal that the B-doping onto 2D MXene nanosheets can largely improve the intermediate H* adsorption kinetics and reduce the charge-transfer resistance toward the HER, leading to increased reactivity of active sites and favorable electrode kinetics. Importantly, the newly designed electrocatalyst based on Ru nanoparticles supported on B-doped MXene (Ru@B-Ti3 C2 Tx ) nanosheets shows a remarkable catalytic activity with low overpotentials of 62.9 and 276.9 mV to drive 10 and 100 mA cm-2 , respectively, for the HER, while exhibiting excellent cycling stabilities. Moreover, according to the theoretical calculations, Ru@B-Ti3 C2 Tx exhibits a near-zero value of Gibbs free energy (ΔGH*  = 0.002 eV) for the HER. This work introduces a facile strategy to functionalize MXene for use as a solid support for efficient electrocatalysts.

1D-2D Synergistic MXene-Nanotubes Hybrids for Efficient Perovskite Solar Cells.

Incorporation of 2D MXenes into the electron transporting layer (ETL) of perovskite solar cells (PSCs) has been shown to deliver high-efficiency photovoltaic (PV) devices. However, the ambient fabrication of the ETLs leads to unavoidable deterioration in the electrical properties of MXene due to oxidation. Herein, sorted metallic single-walled carbon nanotubes (m-SWCNTs) are employed to prepare MXene/SWCNTs composites to improve the PV performance of PSCs. With the optimized composition, a power conversion efficiency of over 21% is achieved. The improved photoluminescence and reduced charge transfer resistance revealed by electrochemical impedance spectroscopy demonstrated low trap density and improved charge extraction and transport characteristics due to the improved conductivity originating from the presence of nanotubes as well as the reduced defects associated with oxygen vacancies on the surface of the SnO2 . The MXene/SWCNTs strategy reported here provides a new avenue for realizing high-performance PSCs.

Doping Strategies in Sb2 S3 Thin Films for Solar Cells.

Sb2 S3 is an attractive solar absorber material that has garnered tremendous interest because of its fascinating properties for solar cells including suitable band gap, high absorption coefficient, earth abundance, and excellent stability. Over the past several years, intensive efforts have been made to enhance the photovoltaic efficiencies of Sb2 S3 solar cells using many promising approaches including interfacial engineering, surface passivation, additive engineering, and band-gap engineering of the charge transport layers and active light absorbing Sb2 S3 materials. Recently, doping strategies in Sb2 S3 light absorbers have gained attention as they promise to play important roles in controlling band gap, regulating film morphology, and passivating grain boundaries, and thus resulting in enhanced carrier transport, which is one of the most challenging issues in this cutting-edge research field. In this review, after a brief introduction to Sb2 S3 , an overview of Sb2 S3 solar cells and their fundamental properties are provided. Recent advances in doping strategies in Sb2 S3 thin films and solar cells are then discussed to provide in-depth understanding of the effects of various dopants on the photovoltaic properties of Sb2 S3 materials. In conclusion, the personal perspectives and outlook to the future development of Sb2 S3 solar cells are provided.

Breaking Platinum Nanoparticles to Single-Atomic Pt-C4 Co-catalysts for Enhanced Solar-to-Hydrogen Conversion.

Effective transfer and utilization of the photogenerated electrons are a key factor for achieving highly efficient H2 generation by photocatalytic water splitting. Apart from the activity of the co-catalyst, the interface between the co-catalyst and semiconductor is of particular importance. Guided by DFT calculations, single-atom (SA) Pt doped carbon nitride (CN) is successfully synthesized for use as the co-catalyst to the semiconducting CuS. The catalyst system (Pt1-CN@CuS) exhibits an enhanced photocatalytic performance for water splitting with a H2 production rate of 25.4 µmol h-1 and an apparent quantum yield (AQY) of 50.3 % under the illumination of LED-530. Solar-to-hydrogen (STH) conversion efficiency is calculated to be 0.5 % under AM 1.5 illumination. This is the very first investigation of SA as the co-catalyst, which decreases the overpotential of CN during the water splitting and lowers interfacial resistance of the catalyst/co-catalyst and co-catalyst/electrolyte.

Unsaturated p-Metal-Based Metal-Organic Frameworks for Selective Nitrogen Reduction under Ambient Conditions.

Electrochemical ammonia synthesis that utilizes renewable electricity in the nitrogen reduction reaction (NRR) has recently been remarkably considered. Of particular importance is to develop efficient electrocatalysts at low costs. Herein, highly selective nitrogen capture using porous aluminum-based metal-organic frameworks (MOFs) materials, MIL-100 (Al), is first designed for the electrochemical nitrogen fixation in alkaline media under ambient conditions. Owing to the unique structure, MIL-100 (Al) exhibits remarkable NRR properties (NH3 yield: 10.6 µg h-1 cm-2 mgcat.-1 and Faradaic efficiency: 22.6%) at a low overpotential (177 mV). Investigation indicates that the catalyst shows excellent N2-selective captures due to the unsaturated metal sites binding with N2. More specifically, as the Al 3p band can strongly interact with N 2p orbitals, Al as a main group metal presents a high and selective affinity to N2. The utilization of multifunctional MOF catalysts delivers both high N2 selectivity and abundant catalytic sites, resulting in remarkable efficiency for NH3 production.

Recent Advances in Perovskite-Based Building-Integrated Photovoltaics.

Perovskite-based solar cells have attracted great attention due to their low cost and high photovoltaic (PV) performance. In addition to their success in the PV sector, there has been growing interest in employing perovskites in energy-efficient smart windows and other building technologies owing to their large absorption coefficient and color tunability. The major challenge lies in integrating perovskite materials into windows and building facades and combining them with added functionalities while maintaining their remarkable power conversion efficiencies. Herein, advances that have been made in the application of perovskites to building-integrated photovoltaics (BIPVs) in four areas are highlighted: semitransparent windows, colorful wall facades, electrochromic windows, and thermochromic windows. In addition, the opportunities and challenges of this cutting-edge research area and important roadmaps for the future use of perovskites in BIPVs are discussed.

Advances in Emerging Solar Cells.

There has been a continuous increase in the world's electricity generation and consumption over the years [...].

Efficiency and stability enhancement of perovskite solar cells using reduced graphene oxide derived from earth-abundant natural graphite.

Graphene - two-dimensional (2D) sheets of carbon atoms linked in a honeycomb pattern - has unique properties that exhibit great promise for various applications including solar cells. Herein we prepared two-dimensional (2D) reduced graphene oxide (rGO) nanosheets from naturally abundant graphite flakes (obtained from Tuv aimag in Mongolia) using solution processed chemical oxidation and thermal reduction methods. As a proof of concept, we used our rGO as a hole transporting material (HTM) in perovskite solar cells (PSCs). Promisingly, the use of rGO in the hole transporting layer (HTL) not only enhanced the photovoltaic efficiency of PSCs, but also improved the device stability. In particular, the best performing PSC employing rGO nanosheets exhibited a power conversion efficiency (PCE) of up to 18.13%, while the control device without rGO delivered a maximum efficiency of 17.26%. The present work demonstrates the possibilities for solving PSC issues (stability) using nanomaterials derived from naturally abundant graphite sources.

A luminescent terbium coordination complex as multifunctional sensing platform.

In this paper, we report the synthesis of a multifunctional fluorescent probe Tb-CP, Tb(HL)(EtOH)2(NO3)2 (HPU-10) (H2L = 2,6-bis-(5-pyridin-4-yl-1H-[1,2,4]triazol-3-yl)- pyridine), and demonstrate that this novel chemosensor has the property of ratiometric detection of Zn2+ and Cd2+. The detection limit of HPU-10 sensing Zn2+ and Cd2+ is 0.319 and 0.965 µM, respectively. The sensing mechanism can be explained by (i) the decomposition of HPU-10 and (ii) the recombination of Zn2+ or Cd2+ with ligand forming 2HL--Zn2+ or 2HL--Cd2+, respectively. Moreover, the fluorescent sensor HPU-10 can detect the nitroaromatic compound 2, 4-DNP via a fluorescence quenching mechanism. The detection limits obtained from linear regression curve plots of 2, 4-DNP is calculated to be 1.69 µM. In addition, the possible use of the probe coated paper for tracing the target analytes has also been presented.

Surface-Halogenation-Induced Atomic-Site Activation and Local Charge Separation for Superb CO2 Photoreduction.

Solar-energy-driven CO2 conversion into value-added chemical fuels holds great potential in renewable energy generation. However, the rapid recombination of charge carriers and deficient reactive sites, as two major obstacles, severely hampers the photocatalytic CO2 reduction activity. Herein, a desirable surface halogenation strategy to address the aforementioned concerns over a Sillén-related layer-structured photocatalyst Bi2 O2 (OH)(NO3 ) (BON) is demonstrated. The surface halogen ions that are anchored on the Bi atoms by replacing surface hydroxyls on the one hand facilitate the local charge separation, and, on the other hand, activate the hydroxyls that profoundly boost the adsorption of CO2 molecules and protons and facilitate the CO2 conversion process, as evidenced by experimental and theoretical results collectively. Among the three series of BON-X (X = Cl, Br, and I) catalysts, BON-Br shows the most substantially enhanced CO production rate (8.12 µmol g-1 h-1 ) without any sacrificial agents or cocatalysts, ≈73 times higher than that of pristine Bi2 O2 (OH)(NO3 ), also exceeding that of the state-of-the-art photocatalysts reported to date. This work presents a surface polarization protocol for engineering charge behavior and reactive sites to promote photocatalysis, which shows great promise to the future design of high-performance materials for clean energy production.

Electrically Sorted Single-Walled Carbon Nanotubes-Based Electron Transporting Layers for Perovskite Solar Cells.

Incorporation of as prepared single-walled carbon nanotubes (SWCNTs) into the electron transporting layer (ETL) is an effective strategy to enhance the photovoltaic performance of perovskite solar cells (PSCs). However, the fundamental role of the SWCNT electrical types in the PSCs is not well understood. Herein, we prepared semiconducting (s-) and metallic (m-) SWCNT families and integrated them into TiO2 photoelectrodes of the PSCs. Based on experimental and theoretical studies, we found that the electrical type of the nanotubes plays an important role in the devices. In particular, the mixture of s-SWCNTs and m-SWCNTs (2:1 w/w)-based PSCs exhibited a remarkable efficiency of up to 19.35%, which was significantly higher than that of the best control cell (17.04%). In this class of PSCs, semiconducting properties of s-SWCNTs play a critical role in extracting and transporting electrons, whereas m-SWCNTs provide high conductance throughout the electrode.

Near-Infrared Active Lead Chalcogenide Quantum Dots: Preparation, Post-Synthesis Ligand Exchange, and Applications in Solar Cells.

Quantum dots (QDs) of lead chalcogenides (e.g. PbS, PbSe, and PbTe) are attractive near-infrared (NIR) active materials that show great potential in a wide range of applications, such as, photovoltaics (PV), optoelectronics, sensors, and bio-electronics. The surface ligand plays an essential role in the production of QDs, post-synthesis modification, and their integration to practical applications. Therefore, it is critically important that the influence of surface ligands on the synthesis and properties of QDs is well understood for their applications in various devices. In this Review we elaborate the application of colloidal synthesis techniques for the preparation of lead chalcogenide based QDs. We specifically focus on the influence of surface ligands on the synthesis of QDs and their solution-phase ligand exchange. Given the importance of lead chalcogenide QDs as potential light harvesters, we also pay particular attention to the current progress of these QDs in photovoltaic applications.

Synthesis, purification, properties and characterization of sorted single-walled carbon nanotubes.

Single-walled carbon nanotubes (SWCNTs) have attracted significant attention due to their outstanding mechanical, chemical and optoelectronic properties, which makes them promising candidates for use in a wide range of applications. However, as-produced SWCNTs have a wide distribution of various chiral species with different properties (i.e. electronic structures). In order to take full advantage of SWCNT properties, highly purified and well-separated SWCNTs are of great importance. Recent advances have focused on developing new strategies to effectively separate nanotubes into single-chirality and/or semiconducting/metallic species and integrating them into different applications. This review highlights recent progress in this cutting-edge research area alongside the enormous development of their identification and structural characterization techniques. A comprehensive review of advances in both controlled synthesis and post-synthesis separation methods of SWCNTs are presented. The relationship between the unique structure of SWCNTs and their intrinsic properties is also discussed. Finally, important future directions for the development of sorting and purification protocols for SWCNTs are provided.