Titanium Carbide (Ti3C2Tx) MXene for Sequestration of Aquatic Pollutants.

The rapid expansion of industrialization has resulted in the release of multiple ecological contaminants in gaseous, liquid, and solid forms, which pose significant environmental risks to many different ecosystems. The efficient and cost-effective removal of these environmental pollutants has attracted global attention. This growing concern has prompted the synthesis and optimization of nanomaterials and their application as potential pollutant removal. In this context, MXene is considered an outstanding photocatalytic candidate due to its unique physicochemical and mechanical properties, which include high specific surface area, physiological compatibility, and robust electrodynamics. This review highlights recent advances in shaping titanium carbide (Ti3C2Tx) MXenes, emphasizing the importance of termination groups to boost photoactivity and product selectivity, with a primary focus on engineering aspects. First, a broad overview of Ti3C2Tx MXene is provided, delving into its catalytic properties and the formation of surface termination groups to establish a comprehensive understanding of its fundamental catalytic structure. Subsequently, the effects of engineering the morphology of Ti3C2Tx MXene into different structures, such as two-dimensional (2D) accordion-like forms, monolayers, hierarchies, quantum dots, and nanotubes. Finally, a concise overview of the removal of different environmental pollutants is presented, and the forthcoming challenges, along with their prospective outlooks, are delineated.

Dimensionality engineering of metal halide perovskites.

Metal halide perovskites are a class of materials that are ideal for photodetectors and solar cells due to their excellent optoelectronic properties. Their low-cost and low temperature synthesis have made them attractive for extensive research aimed at revolutionizing the semiconductor industry. The rich chemistry of metal halide perovskites allows compositional engineering resulting in facile tuning of the desired optoelectronic properties. Moreover, using different experimental synthesis and deposition techniques such as solution processing, chemical vapor deposition and hot-injection methods, the dimensionality of the perovskites can be altered from 3D to 0D, each structure opening a new realm of applications due to their unique properties. Dimensionality engineering includes both morphological engineering-reducing the thickness of 3D perovskite into atomically thin films-and molecular engineering-incorporating long-chain organic cations into the perovskite mixture and changing the composition at the molecular level. The optoelectronic properties of the perovskite structure including its band gap, binding energy and carrier mobility depend on both its composition and dimensionality. The plethora of different photodetectors and solar cells that have been made with different compositions and dimensions of perovskite will be reviewed here. We will conclude our review by discussing the kinetics and dynamics of different dimensionalities, their inherent stability and toxicity issues, and how reaching similar performance to 3D in lower dimensionalities and their large-scale deployment can be achieved.

Surpassing the Exciton Diffusion Limit in Single-Walled Carbon Nanotube Sensitized Solar Cells.

Semiconducting single-walled carbon nanotube (s-SWNT) light sensitized devices, such as infrared photodetectors and solar cells, have recently been widely reported. Despite their excellent individual electrical properties, efficient carrier transport from one carbon nanotube to another remains a fundamental challenge. Specifically, photovoltaic devices with active layers made from s-SWNTs have suffered from low efficiencies caused by three main challenges: the overwhelming presence of high-bandgap polymers in the films, the weak bandgap offset between the LUMO of the s-SWNTs and the acceptor C60, and the limited exciton diffusion length from one SWNT to another of around 5 nm that limits the carrier extraction efficiency. Herein, we employ a combination of processing and device architecture design strategies to address each of these transport challenges and fabricate photovoltaic devices with s-SWNT films well beyond the exciton diffusion limit of 5 nm. While our solution processing method minimizes the presence of undesired polymers in our active films, our interfacial designs led to a significant increase in current generation with the addition of a highly doped C60 layer (n-doped C60), resulting in increased carrier separation efficiency from the s-SWNTs films. We create a dense interconnected nanoporous mesh of s-SWNTs using solution shearing and infiltrate it with the acceptor C60. Thus, our final engineered bulk heterojunction allows carriers from deep within to be extracted by the C60 registering a 10-fold improvement in performance from our preliminary structures.

Mechanically Durable and Highly Stretchable Transistors Employing Carbon Nanotube Semiconductor and Electrodes.

Mechanically durable stretchable trans-istors are fabricated using carbon nanotube electrical components and tough thermoplastic elastomers. After an initial conditioning step, the electrical characteristics remain constant with strain. The strain-dependent characteristics are similar in orthogonal stretching directions. Devices can be impacted with a hammer and punctured with a needle while remaining functional and stretchable.

High-yield sorting of small-diameter carbon nanotubes for solar cells and transistors.

We describe herein a high-yield method to selectively disperse semiconducting CoMoCAT (CO disproportionation on Co-Mo catalysts) single-walled carbon nanotubes (SWNTs) with regioregular poly(3-alkylthiophenes) polymers. We observed that the dispersion yield was directly related to the length of the polymer's alkyl side chains. Molecular dynamics simulations in explicit toluene (real toluene molecules) indicate that polythiophenes with longer alkyl side chains bind strongly to SWNTs, due to the increased overall surface contact area with the nanotube. Furthermore, the sorting process selectively enriches smaller-diameter CoMoCAT SWNTs with larger bandgaps, which is ideal for solar cell applications. Compared to the larger diameter sorted HiPco (High-Pressure CO) SWNTs, solar cells fabricated using our sorted CoMoCAT SWNTs demonstrated higher open-circuit voltage (Voc) and infrared external quantum efficiency (EQE). The Voc achieved is the highest reported for solar cells based on SWNT absorbers under simulated AM1.5 solar illumination. Additionally, we employed the sorted CoMoCAT SWNTs to fabricate thin film transistors with excellent uniformity and device performance.

Folded-light-path colloidal quantum dot solar cells.

Colloidal quantum dot photovoltaics combine low-cost solution processing with quantum size-effect tuning to match absorption to the solar spectrum. Rapid advances have led to certified solar power conversion efficiencies of over 7%. Nevertheless, these devices remain held back by a compromise in the choice of quantum dot film thickness, balancing on the one hand the need to maximize photon absorption, mandating a thicker film, and, on the other, the need for efficient carrier extraction, a consideration that limits film thickness. Here we report an architecture that breaks this compromise by folding the path of light propagating in the colloidal quantum dot solid. Using this method, we achieve a substantial increase in short-circuit current, ultimately leading to improved power conversion efficiency.

Self-assembled, nanowire network electrodes for depleted bulk heterojunction solar cells.

Herein, a solution-processed, bottom-up-fabricated, nanowire network electrode is developed. This electrode features a ZnO template which is converted into locally connected, infiltratable, TiO2 nanowires. This new electrode is used to build a depleted bulk heterojunction solar cell employing hybrid-passivated colloidal quantum dots. The new electrode allows the application of a thicker, and thus more light-absorbing, colloidal quantum dot active layer, from which charge extraction of an efficiency comparable to that obtained from a thinner, planar device could be obtained.

Graded recombination layers for multijunction photovoltaics.

Multijunction devices consist of a stack of semiconductor junctions having bandgaps tuned across a broad spectrum. In solar cells this concept is used to increase the efficiency of photovoltaic harvesting, while light emitters and detectors use it to achieve multicolor and spectrally tunable behavior. In series-connected current-matched multijunction devices, the recombination layers must allow the hole current from one cell to recombine, with high efficiency and low voltage loss, with the electron current from the next cell. We recently reported a tandem solar cell in which the recombination layer was implemented using a progression of n-type oxides whose doping densities and work functions serve to connect, with negligible resistive loss at solar current densities, the constituent cells. Here we present the generalized conditions for design of efficient graded recombination layer solar devices. We report the number of interlayers and the requirements on work function and doping of each interlayer, to bridge an work function difference as high as 1.6 eV. We also find solutions that minimize the doping required of the interlayers in order to minimize optical absorption due to free carriers in the graded recombination layer (GRL). We demonstrate a family of new GRL designs experimentally and highlight the benefits of the progression of dopings and work functions in the interlayers.

A donor-supply electrode (DSE) for colloidal quantum dot photovoltaics.

The highest-performing colloidal quantum dot (CQD) photovoltaics (PV) reported to date have relied on high-temperature (>500°C) annealing of electron-accepting TiO2. Room-temperature processing reduces energy payback time and manufacturing cost, enables flexible substrates, and permits tandem solar cells that integrate a small-bandgap back cell atop a low-thermal-budget larger-bandgap front cell. Here we report an electrode strategy that enables a depleted-heterojunction CQD PV device to be fabricated entirely at room temperature. We find that simply replacing the high-temperature-processed TiO2 with a sputtered version of the same material leads to poor performance due to the low mobility of the sputtered oxide. We develop instead a two-layer donor-supply electrode (DSE) in which a highly doped, shallow work function layer supplies a high density of free electrons to an ultrathin TiO2 layer via charge-transfer doping. Using the DSE we build all-room-temperature-processed small-bandgap (1 eV) colloidal quantum dot solar cells having 4% solar power conversion efficiency and high fill factor. These 1 eV bandgap cells are suitable for use as the back junction in tandem solar cells. The DSE concept, combined with control over TiO2 stoichiometry in sputtering, provides a much-needed tunable electrode to pair with quantum-size-effect CQD films.

Enhanced open-circuit voltage in visible quantum dot photovoltaics by engineering of carrier-collecting electrodes.

Colloidal quantum dots (CQDs) enable multijunction solar cells using a single material programmed using the quantum size effect. Here we report the systematic engineering of 1.6 eV PbS CQD solar cells, optimal as the front cell responsible for visible-wavelength harvesting in tandem photovoltaics. We rationally optimize each of the device's collecting electrodes-the heterointerface with electron-accepting TiO(2) and the deep-work-function hole-collecting MoO(3) for ohmic contact-for maximum efficiency. We report an open-circuit voltage of 0.70 V, the highest observed in a colloidal quantum dot solar cell operating at room temperature. We report an AM1.5 solar power conversion efficiency of 3.5%, the highest observed in >1.5 eV bandgap CQD PV device.

Electron acceptor materials engineering in colloidal quantum dot solar cells.

Lead sulfide colloidal quantum dot (CQD) solar cells with a solar power conversion efficiency of 5.6% are reported. The result is achieved through careful optimization of the titanium dioxide electrode that serves as the electron acceptor. Metal-ion-doped sol-gel-derived titanium dioxide electrodes produce a tunable-bandedge, well-passivated materials platform for CQD solar cell optimization.

Efficient, stable infrared photovoltaics based on solution-cast colloidal quantum dots.

Half of the sun's power lies in the infrared. As a result, the optimal bandgaps for solar cells in both the single-junction and even the tandem architectures lie beyond 850 nm. However, progress in low-cost, large-area, physically flexible solar cells has instead been made in organic and polymer materials possessing absorption onsets in the visible. Recent advances have been achieved in solution-cast infrared photovoltaics through the use of colloidal quantum dots. Here we report stable solution-processed photovoltaic devices having 3.6% power conversion efficiency in the infrared. The use of a strongly bound bidentate linker, benzenedithiol, ensures device stability over weeks. The devices reach external quantum efficiencies of 46% in the infrared and 70% across the visible. We investigate in detail the physical mechanisms underlying the operation of this class of device. In contrast with drift-dominated behavior in recent reports of PbS quantum dot photovoltaics, we find that diffusion of electrons and holes over hundreds of nanometers through our PbSe colloidal quantum dot solid is chiefly responsible for the high external quantum efficiencies obtained in this new class of devices.