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Showing papers by "Peidong Yang published in 2020"


Journal ArticleDOI
TL;DR: This Review presents the surface and interface control of nanoparticle catalysts in the context of oxygen reduction reaction (ORR), electrochemical CO2 reduction Reaction (CO2 RR), and tandem catalysis in three sections.
Abstract: The surface and interfaces of heterogeneous catalysts are essential to their performance as they are often considered to be active sites for catalytic reactions. With the development of nanoscience, the ability to tune surface and interface of nanostructures has provided a versatile tool for the development and optimization of a heterogeneous catalyst. In this Review, we present the surface and interface control of nanoparticle catalysts in the context of oxygen reduction reaction (ORR), electrochemical CO2 reduction reaction (CO2 RR), and tandem catalysis in three sections. In the first section, we start with the activity of ORR on the nanoscale surface and then focus on the approaches to optimize the performance of Pt-based catalyst including using alloying, core-shell structure, and high surface area open structures. In the section of CO2 RR, where the surface composition of the catalysts plays a dominant role, we cover its reaction fundamentals and the performance of different nanosized metal catalysts. For tandem catalysis, where adjacent catalytic interfaces in a single nanostructure catalyze sequential reactions, we describe its concept and principle, catalyst synthesis methodology, and application in different reactions.

401 citations


Journal ArticleDOI
29 Apr 2020-Nature
TL;DR: An effective strategy to substantially inhibit in-plane ion diffusion in two-dimensional halide perovskites by incorporating rigid π-conjugated organic ligands is reported and highly stable and tunable lateral epitaxial heterostructures, multiheterostructureures and superlattices are demonstrated.
Abstract: Epitaxial heterostructures based on oxide perovskites and III–V, II–VI and transition metal dichalcogenide semiconductors form the foundation of modern electronics and optoelectronics1–7. Halide perovskites—an emerging family of tunable semiconductors with desirable properties—are attractive for applications such as solution-processed solar cells, light-emitting diodes, detectors and lasers8–15. Their inherently soft crystal lattice allows greater tolerance to lattice mismatch, making them promising for heterostructure formation and semiconductor integration16,17. Atomically sharp epitaxial interfaces are necessary to improve performance and for device miniaturization. However, epitaxial growth of atomically sharp heterostructures of halide perovskites has not yet been achieved, owing to their high intrinsic ion mobility, which leads to interdiffusion and large junction widths18–21, and owing to their poor chemical stability, which leads to decomposition of prior layers during the fabrication of subsequent layers. Therefore, understanding the origins of this instability and identifying effective approaches to suppress ion diffusion are of great importance22–26. Here we report an effective strategy to substantially inhibit in-plane ion diffusion in two-dimensional halide perovskites by incorporating rigid π-conjugated organic ligands. We demonstrate highly stable and tunable lateral epitaxial heterostructures, multiheterostructures and superlattices. Near-atomically sharp interfaces and epitaxial growth are revealed by low-dose aberration-corrected high-resolution transmission electron microscopy. Molecular dynamics simulations confirm the reduced heterostructure disorder and larger vacancy formation energies of the two-dimensional perovskites in the presence of conjugated ligands. These findings provide insights into the immobilization and stabilization of halide perovskite semiconductors and demonstrate a materials platform for complex and molecularly thin superlattices, devices and integrated circuits. An epitaxial growth strategy that improves the stability of two-dimensional halide perovskites by inhibiting ion diffusion in their heterostructures using rigid π-conjugated ligands is demonstrated, and shows near-atomically sharp interfaces.

228 citations


Journal ArticleDOI
01 Mar 2020
TL;DR: In this article, the authors illustrate the evolution and advances of photosynthetic semiconductor biohybrid focusing on the conversion of CO2 to value-added chemicals, and discuss the advantageous coupling of electrotrophic organisms with light-active electrodes for solar-to-chemical conversion.
Abstract: Photosynthetic semiconductor biohybrids integrate the best attributes of biological whole-cell catalysts and semiconducting nanomaterials. Enzymatic machinery enveloped in its native cellular environment offers exquisite product selectivity and low substrate activation barriers while semiconducting nanomaterials harvest light energy stably and efficiently. In this Review Article, we illustrate the evolution and advances of photosynthetic semiconductor biohybrids focusing on the conversion of CO2 to value-added chemicals. We begin by considering the potential of this nascent field to meet global energy challenges while comparing it to alternate approaches. This is followed by a discussion of the advantageous coupling of electrotrophic organisms with light-active electrodes for solar-to-chemical conversion. We detail the dynamic investigation of photosensitized microorganisms creating direct light harvesting within unicellular organisms while describing complementary developments in the understanding of charge transfer mechanisms and cytoprotection. Lastly, we focus on trends and improvements needed in photosynthetic semiconductor biohybrids in order to address future challenges and enhance their widespread adoption for the production of solar chemicals. Artificial photosynthetic technologies could potentially contribute to limiting global warming while providing useful chemicals for society. This Review Article covers photosynthetic semiconductor biohybrids—electrodes/nanomaterials coupled with microorganisms—for light-driven catalytic conversion of CO2 to fuels and other value-added chemicals.

191 citations


Journal ArticleDOI
19 Aug 2020-Joule
TL;DR: In this paper, the authors show that a Cu-Ag tandem catalyst on a gas diffusion electrode (GDE) can enhance the C2+ production rate from CO2 through CO2 reduction to CO on Ag and subsequent carbon coupling on Cu.

167 citations


Journal ArticleDOI
TL;DR: This work provides an effective strategy to produce high-performance Pt-Co nanoframes for fuel-cell-related applications and indicates that the weakened binding of intermediate carbonaceous poison contributes to the enhanced MOR activity.
Abstract: Pt-based alloy catalysts are promising candidates for fuel-cell applications, especially for cathodic oxygen reduction reaction (ORR) and anodic methanol oxidation reaction (MOR). The rational design of composition and morphology is crucial to promoting catalytic performances. Here, we report the synthesis of Pt-Co nanoframes via chemical etching of Co from solid rhombic dodecahedra. The obtained Pt-Co nanoframes exhibit excellent ORR mass activity in acidic electrolyte, which is as high as 0.40 A mgPt-1 initially and 0.34 A mgPt-1 after 10 000 potential cycles at 0.95 VRHE. Furthermore, their MOR mass activity in alkaline media is up to 4.28 A mgPt-1 and is 4-fold higher than that of commercial Pt/C catalyst. Experimental studies indicate that the weakened binding of intermediate carbonaceous poison contributes to the enhanced MOR behavior. More impressively, the Pt-Co nanoframes also demonstrate remarkable stability under long-term testing, which could be attributed to the negligible electrochemical Co dissolution.

127 citations


Journal ArticleDOI
15 Apr 2020-Joule
TL;DR: In this article, the authors investigated the microorganism-cathode interface and found that tuning the bulk electrolyte pH and increasing its buffering capacity supported the formation of a close-packed nanowire-bacteria cathode.

101 citations


Journal ArticleDOI
TL;DR: The solution phase synthesis of single-crystalline CsEuCl3 nanocrystals with a uniform size distribution centered around 15 nm are demonstrated, which represent a promising candidate to replace lead halide perovskites.
Abstract: Because of the toxicity of lead, searching for a lead-free halide perovskite semiconducting material with comparable optical and electronic properties is of great interest. Rare-earth-based halide perovskite represents a promising class of materials for this purpose. In this work, we demonstrate the solution-phase synthesis of single-crystalline CsEuCl3 nanocrystals with a uniform size distribution centered around 15 nm. The CsEuCl3 nanocrystals have photoluminescence emission centered at 435 nm, with a full width at half-maximum of 19 nm. Furthermore, CsEuCl3 nanocrystals can be embedded in a polymer matrix that provides enhanced stability under continuous laser irradiation. Lead-free rare-earth cesium europium halide perovskite nanocrystals represent a promising candidate to replace lead halide perovskites.

81 citations


Journal ArticleDOI
TL;DR: It is indicated that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.
Abstract: Achieving perovskite-based high-color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high-color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr6]4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

77 citations


Journal ArticleDOI
TL;DR: In this paper, a nanoparticle/ordered-ligand interlayer was proposed for high-specificity CO2 electrocatalysis, which consists of a metal nanoparticle surface and a detached layer of ligands in its vicinity.
Abstract: Enzymes feature the concerted operation of multiple components around an active site, leading to exquisite catalytic specificity. Realizing such configurations on synthetic catalyst surfaces remains elusive. Here, we report a nanoparticle/ordered-ligand interlayer that contains a multi-component catalytic pocket for high-specificity CO2 electrocatalysis. The nanoparticle/ordered-ligand interlayer comprises a metal nanoparticle surface and a detached layer of ligands in its vicinity. This interlayer possesses unique pseudocapacitive characteristics where desolvated cations are intercalated, creating an active-site configuration that enhances catalytic turnover by two orders and one order of magnitude against a pristine metal surface and nanoparticle with tethered ligands, respectively. The nanoparticle/ordered-ligand interlayer is demonstrated across several metals with up to 99% CO selectivity at marginal overpotentials and onset overpotentials of as low as 27 mV, in aqueous conditions. Furthermore, in a gas-diffusion environment with neutral media, the nanoparticle/ordered-ligand interlayer achieves nearly unit CO selectivity at high current densities (98.1% at 400 mA cm−2). The complex, multi-component environments found in enzymes induce high catalytic specificity, but are difficult to achieve in synthetic catalysts. Now, researchers report a catalyst comprising a dynamic, ordered layer of ligands above a nanoparticle surface that creates a pocket to facilitate CO2 electroreduction.

75 citations


Journal ArticleDOI
TL;DR: It is suggested that disordered copper structures facilitate C–C bond formation from CO2 and that electrochemical nanocrystal scrambling is an avenue toward creating such catalysts.
Abstract: Promotion of C-C bonds is one of the key fundamental questions in the field of CO2 electroreduction. Much progress has occurred in developing bulk-derived Cu-based electrodes for CO2-to-multicarbons (CO2-to-C2+), especially in the widely studied class of high-surface-area "oxide-derived" copper. However, fundamental understanding into the structural characteristics responsible for efficient C-C formation is restricted by the intrinsic activity of these catalysts often being comparable to polycrystalline copper foil. By closely probing a Cu nanoparticle (NP) ensemble catalyst active for CO2-to-C2+, we show that bias-induced rapid fusion or "electrochemical scrambling" of Cu NPs creates disordered structures intrinsically active for low overpotential C2+ formation, exhibiting around sevenfold enhancement in C2+ turnover over crystalline Cu. Integrating ex situ, passivated ex situ, and in situ analyses reveals that the scrambled state exhibits several structural signatures: a distinct transition to single-crystal Cu2O cubes upon air exposure, low crystallinity upon passivation, and high mobility under bias. These findings suggest that disordered copper structures facilitate C-C bond formation from CO2 and that electrochemical nanocrystal scrambling is an avenue toward creating such catalysts.

72 citations


Journal ArticleDOI
14 Sep 2020
TL;DR: A new generation of semiconducting materials based on metal halide perovskites has recently been launched into the scientific spotlight, exhibiting outstanding optoelectronic properties as discussed by the authors.
Abstract: ConspectusA new generation of semiconducting materials based on metal halide perovskites has recently been launched into the scientific spotlight, exhibiting outstanding optoelectronic properties a...

Journal ArticleDOI
20 Feb 2020-ACS Nano
TL;DR: This large-scale patterning method enables the patterning of single crystal cesium lead halide perovskite arrays with tunable spacing and crystal size in high production yield and renders a platform for study of fundamental properties and opportunities for novel perovkite-based optoelectronic applications.
Abstract: Halide perovskites have many important optoelectronic properties, including high emission efficiency, high absorption coefficients, color purity, and tunable emission wavelength, which makes these materials promising for optoelectronic applications. However, the inability to precisely control large-scale patterned growth of halide perovskites limits their potential toward various device applications. Here, we report a patterning method for the growth of a cesium lead halide perovskite single crystal array. Our approach consists of two steps: (1) cesium halide salt arrays patterning and (2) chemical vapor transport process to convert salt arrays into single crystal perovskite arrays. Characterizations including energy-dispersive X-ray spectroscopy and photoluminescence have been employed to confirm the chemical compositions and the optical properties of the as-synthesized perovskite arrays. This patterning method enables the patterning of single crystal cesium lead halide perovskite arrays with tunable spacing (from 2 to 20 μm) and crystal size (from 200 nm to 1.2 μm) in high production yield (almost every pixel in the array is successfully grown with converted perovskite crystals). Our large-scale patterning method renders a platform for the study of fundamental properties and opportunities for perovskite-based optoelectronic applications.

Journal ArticleDOI
05 Aug 2020
TL;DR: In this article, the authors used in situ nanoscale cathodoluminescence microscopy with low electron beam exposure to visualize nucleation and growth in the thermally driven transition to the perovskite phase in hundreds of non-perovskites phase nanowires.
Abstract: Summary Microscopic pathways of structural phase transitions in metal halide perovskites are difficult to probe because they occur over disparate time and length scales and because electron-based microscopies typically used to directly probe nanoscale dynamics of phase transitions often damage metal halide perovskite materials. Using in situ nanoscale cathodoluminescence microscopy with low electron beam exposure, we visualize nucleation and growth in the thermally driven transition to the perovskite phase in hundreds of non-perovskite phase nanowires. In combination with molecular dynamics simulations, we reveal that the transformation does not follow a simple martensitic mechanism, but proceeds despite a substantial energy barrier via ion diffusion through a liquid-like interface between the two structures. While cations are disordered in this liquid-like region, the halide ions retain substantial spatial correlations. This detailed picture not only reveals how phase transitions between disparate structures can proceed, but also opens the possibility to control such processes.

Posted ContentDOI
29 Dec 2020
TL;DR: It is argued for an integrated biomanufacturing plant replete with modules for microbial resource utilization, production, and recycling of food, pharmaceuticals, and biomaterials required for sustaining future intrepid astronauts.
Abstract: A crewed mission to and from Mars may include an exciting array of enabling biotechnologies that leverage inherent mass, power, and volume advantages over traditional abiotic approaches. In this perspective, we articulate the scientific and engineering goals and constraints, along with example systems, that guide the design of a surface biomanufactory. Extending past arguments for exploiting stand-alone elements of biology, we argue for an integrated biomanufacturing plant replete with modules for microbial \textit{in situ} resource utilization, production, and recycling of food, pharmaceuticals, and biomaterials required for sustaining future intrepid astronauts. We also discuss aspirational technology trends in each of these target areas in the context of human and robotic exploration missions in the coming century.

Journal ArticleDOI
TL;DR: Using transient absorption microscopy, a polarization-dependent splitting of the band edge exciton line is observed, and from the polarized fluorescence of nanowires in solution, it is determined that the exciton transition dipole moments are anisotropic in strength.
Abstract: Inorganic lead halide perovskite nanostructures show promise as the active layers in photovoltaics, light emitting diodes, and other optoelectronic devices. They are robust in the presence of oxygen and water, and the electronic structure and dynamics of these nanostructures can be tuned through quantum confinement. Here we create aligned bundles of CsPbBr3 nanowires with widths resulting in quantum confinement of the electronic wave functions and subject them to ultrafast microscopy. We directly image rapid one-dimensional exciton diffusion along the nanowires, and we measure an exciton trap density of roughly one per nanowire. Using transient absorption microscopy, we observe a polarization-dependent splitting of the band edge exciton line, and from the polarized fluorescence of nanowires in solution, we determine that the exciton transition dipole moments are anisotropic in strength. Our observations are consistent with a model in which splitting is driven by shape anisotropy in conjunction with long-range exchange.

Journal ArticleDOI
TL;DR: In this article, an amphiphilic block copolymer, polystyrene-block poly(4-vinylpyridine) (PS-P4VP), was introduced to chemically modify the surface of colloidal CsPbBr3 nanowires.
Abstract: The rapid development of solar cells based on lead halide perovskites (LHPs) has prompted very active research activities in other closely-related fields. Colloidal nanostructures of such materials display superior optoelectronic properties. Especially, one-dimensional (1D) LHPs nanowires show anisotropic optical properties when they are highly oriented. However, the ionic nature makes them very sensitive to external environment, limiting their large scale practical applications. Here, we introduce an amphiphilic block copolymer, polystyrene-block-poly(4-vinylpyridine) (PS-P4VP), to chemically modify the surface of colloidal CsPbBr3 nanowires. The resulting core-shell nanowires show enhanced photoluminescent emission and good colloidal stability against water. Taking advantage of the stability enhancement, we further applied a modified Langmuir-Blodgett technique to assemble monolayers of highly aligned nanowires, and studied their anisotropic optical properties.

Journal ArticleDOI
TL;DR: In this article, the size transformation products of the Au22(SG)18 nanocluster under representative working conditions and highlight the surface effect on the transformation kinetics were investigated under thermal and aerobic conditions, the consecutive and pH-dependent transformation from Au22 to both well defined clusters and small Au(I)SR species was identified by ESI-MS and UV-vis spectroscopy.
Abstract: For many applications of well-defined gold nanoclusters, it is desirable to understand their structural evolution behavior under working conditions with molecular precision Here we report the first systematic investigation of the size transformation products of the Au22(SG)18 nanocluster under representative working conditions and highlight the surface effect on the transformation kinetics Under thermal and aerobic conditions, the consecutive and pH-dependent transformation from Au22 to both well-defined clusters and small Au(I)SR species was identified by ESI-MS and UV-vis spectroscopy By introducing a perturbation onto the Au22 surface, significant changes in the activation parameters were determined from the kinetic study of the Au22 transformation This indicates the sensitivity of the nanocluster transformation pathway to the cluster surface The systematic study of cluster transformation and the sensitivity of cluster transformation to the surface revealed herein has significant implications for future attempts to design gold nanoparticles with adaptation to the working environment and the regeneration of active nanoparticles

Journal ArticleDOI
TL;DR: A model system consisting of chemically tunable, highly luminescent halide perovskite nanocrystals is developed to illustrate the role of carrier diffusion and material dimensionality on the carrier recombination kinetics and luminescence efficiency and reveals the scaling laws of photoluminescence quantum yield and radiative lifetime with respect to the aspect ratio of nanocry crystals.
Abstract: Carrier recombination is a crucial process governing the optical properties of a semiconductor. Although various theoretical approaches have been utilized to describe carrier behaviors, a quantitative understanding of the impact of defects and interfaces in low dimensional semiconductor systems is still elusive. Here, we develop a model system consisting of chemically tunable, highly luminescent halide perovskite nanocrystals to illustrate the role of carrier diffusion and material dimensionality on the carrier recombination kinetics and luminescence efficiency. Our advanced synthetic methods provide a well-controlled colloidal system consisting of nanocrystals with different aspect ratios, halide compositions, and surface conditions. Using this system, we reveal the scaling laws of photoluminescence quantum yield and radiative lifetime with respect to the aspect ratio of nanocrystals. The scaling laws derived herein are not only a phenomenological observation but proved a powerful tool disentangling the carrier dynamics of microscopic systems in a quantitative and interpretable manner. The investigation of our model system and theoretical formulation bring to light the dimensionality, as a hidden constraint on carrier dynamics, and identify the diffusion length as an important parameter that distinguishes nanoscale and macroscale carrier behaviors. The conceptual distinction in carrier dynamics in different dimensionality regimes informs new design rules for optical devices where complex microstructures are involved.

Journal ArticleDOI
TL;DR: In this paper, the authors demonstrate the synthesis and study the stability of Cu3Au intermetallic nanowires with long-range atomic ordering, which holds the promise of unique physicochemical properties in many applications.
Abstract: Multimetallic nanowires with long-range atomic ordering hold the promise of unique physicochemical properties in many applications Here we demonstrate the synthesis and study the stability of Cu3Au intermetallic nanowires The synthesis is achieved by using Cu@Au core-shell nanowires as precursors With appropriate Cu/Au stoichiometry, the Cu@Au core-shell nanowires are transformed into fully ordered Cu3Au nanowires under thermal annealing Thermally-driven atom diffusion accounts for this transformation as revealed by X-ray diffraction and electron microscopy studies The twin boundaries abundant in the Cu@Au core-shell nanowires facilitate the ordering process The resulting Cu3Au intermetallic nanowires have uniform and accurate atomic positioning in the crystal lattice, which enhances the nobility of Cu No obvious copper oxides are observed in fully ordered Cu3Au nanowires after annealing in air at 200 °C, a temperature that is much higher than those observed in Cu@Au core-shell and pure Cu nanowires This work opens up an opportunity for further research into the development and applications of intermetallic nanowires

Journal ArticleDOI
TL;DR: Free-standing ultra-thin films of several oxides have been developed, which are mechanically robust and transparent to electrons with Ekin ≥ 200 eV, and to photons, which demonstrate their applicability in environmental X-ray photoelectron and infrared spectroscopy for molecular level studies of solid-gas and solid-liquid interfaces.
Abstract: Free-standing ultrathin (∼2 nm) films of several oxides (Al2O3,TiO2, and others) have been developed, which are mechanically robust and transparent to electrons with Ekin ≥ 200 eV and to photons. We demonstrate their applicability in environmental X-ray photoelectron and infrared spectroscopy for molecular level studies of solid-gas (≥1 bar) and solid-liquid interfaces. These films act as membranes closing a reaction cell and as substrates and electrodes for electrochemical reactions. The remarkable properties of such ultrathin oxides membranes enable atomic/molecular level studies of interfacial phenomena, such as corrosion, catalysis, electrochemical reactions, energy storage, geochemistry, and biology, in a broad range of environmental conditions.

Journal ArticleDOI
Lian Zhang1, Peidong Yang1, Qi Liu1, Jing Wang1, F Yan1, L Duan1, Feng Lin1 
TL;DR: Targeting KLF8-miR-429-SOX2 signaling pathway may provide an effective therapeutic approach to suppress the initiation and progression of OS.
Abstract: Kruppel-like factor 8 (KLF8) regulates critical gene transcription associated with different types of cancer. A novel paradigm in tumor biology suggests that the initiation and progression of osteosarcoma (OS) are driven by osteosarcoma stem cell-like cells (OSCs), but the role and underlying mechanisms of KLF8 in OSCs are poorly elucidated. In this study, an obviously increased level of KLF8 is shown in 9 out of 10 primary OS tissues and is associated with the poor progression-free interval. Significantly, KLF8 expression in CD133+ OSCs is higher than that in CD133- counterparts. By knocking down KLF8 in CD133+ OSCs, we show that si-KLF8-OSCs can hardly form compact spheres. In the meantime, infection with si-KLF8 in CD133+ OSCs results in the downregulation of OCT4 and SOX2; increased adriamycin (ADM) sensitivity; and decreased tumorigenic potential in vivo. Mechanisms study demonstrates that KLF8 directly binds the miR-429 promoter region and regulates its expression transcriptionally. Furthermore, we indicate that miR-429 directly targets SOX2 to mediate cancer stem cell-like features in CD133+ OSCs. In the clinic, miR-429 levels are negatively associated with KLF8 levels in OS, suggesting that an elevated KLF8/miR-429 ratio may have clinical value as a predictive biomarker. In conclusion, targeting the KLF8-miR-429-SOX2 signaling pathway may provide an effective therapeutic approach to suppress the initiation and progression of OS.

Journal ArticleDOI
TL;DR: It is demonstrated that halide ion migration is dependent on the applied electric field and exhibits ionic rectification in this solid-state system, which is due to the nonuniform distribution of the ionic vacancies in the nanowire that results from a competition between electrical screening and their creation/destruction at the electrodes' interfaces.
Abstract: Halide perovskites have attracted increasing research attention with regard to their potential for optoelectronic applications. Because of its low activation energy, ion migration is implicated in the long-term stability and many unusual transport behaviors of halide perovskite devices. However, direct observation and precise control of the ionic transport in halide perovskite crystals remain challenging. Here, we have designed an axial CsPbBr3-CsPbCl3 nanowire heterostructure, in which electric-field-induced halide ion migration was clearly visualized and quantified. We demonstrated that halide ion migration is dependent on the applied electric field and exhibits ionic rectification in this solid-state system, which is due to the nonuniform distribution of the ionic vacancies in the nanowire that results from a competition between electrical screening and their creation/destruction at the electrodes' interfaces. The asymmetric heterostructure characteristics add an additional knob to control the ion movement in the design of advanced ionic circuits with halide perovskites as building blocks.

Journal ArticleDOI
20 May 2020
TL;DR: In this paper, the combination of a Pt-based nanoframe and a metal-organic framework (MOF) is proposed to achieve superior catalytic behavior and multifunctionality.
Abstract: A Pt-based nanoframe is a hollow frame with superior catalytic behavior and a metal−organic framework (MOF) is another porous frame with multifunctionalities. Here, we present the combination of th...

Journal ArticleDOI
TL;DR: In this paper, the phase transition dynamics of metal halide perovskites with anisotropic crystal structures were investigated using in situ optical micro-spectroscopy, showing a large blueshift in the photoluminescence (PL) peak at the low-T/high-T two-phase interface of partially transitioned CsSnI3 and FAPbI3 wires.
Abstract: Triiodide perovskites $${\rm CsPbI}_{3}$$ , $${\rm CsSnI}_{3}$$ , and $${\rm FAPbI}_{3}$$ (where FA is formamidinium) are highly promising materials for a range of optoelectronic applications in energy conversion. However, they are thermodynamically unstable at room temperature, preferring to form low-temperature (low-T) non-perovskite phases with one-dimensional anisotropic crystal structures. While such thermodynamic behavior represents a major obstacle toward realizing high-performance devices based on their high-temperature (high-T) perovskite phases, the underlying phase transition dynamics are still not well understood. Here we use in situ optical micro-spectroscopy to quantitatively study the transition from the low-T to high-T phases in individual $${\rm CsSnI}_{3}$$ and $${\rm FAPbI}_{3}$$ nanowires. We reveal a large blueshift in the photoluminescence (PL) peak (~38 meV) at the low-T/high-T two-phase interface of partially transitioned $${\rm FAPbI}_{3}$$ wire, which may result from the lattice distortion at the phase boundary. Compared to the experimentally derived activation energy of CsSnI3 (~1.93 eV), the activation energy of $${\rm FAPbI}_{3}$$ is relatively small (~0.84 eV), indicating a lower kinetic energy barrier when transitioning from a face-sharing octahedral configuration to a corner-sharing one. Further, the phase propagation rate in CsSnI3 is observed to be relatively high, which may be attributed to a high concentration of Sn vacancies. Our results could not only facilitate a deeper understanding of phase transition dynamics in halide perovskites with anisotropic crystal structures, but also enable controllable manipulation of optoelectronic properties via local phase engineering. Metal halide perovskites are a new class of semiconductors with great promise for a variety of optoelectronic applications. Owing to their soft ionic lattice, halide perovskites often exhibit rich phase transitions between different crystal structures, frequently from the “active” perovskite phases to undesirable “inactive” non-perovskite phases. Understanding and controlling this transition is vital for developing stable, high-performance devices. However, there is limited understanding on how different symmetry, crystal structure, and defect would impact such a phase transition process. In this report, in situ optical micro-spectroscopy is used to systematically investigate the phase transitions from non-perovskite to perovskite phases in individual CsSnI3 and FAPbI3 wires. Compared to the transition from an edge-sharing octahedral non-perovskite structure to a corner-sharing perovskite structure in CsSnI3, the activation energy for the FAPbI3 phase transition is relatively small, indicating a lower energy barrier when starting from a face-sharing octahedral structure in FAPbI3. The high concentration of Sn vacancies is probably responsible for the much higher phase propagation rate in CsSnI3 when compared to a CsPbBrxI3-x system with the same crystal structure but different halide vacancies. Our experimental results expand the knowledge of phase transition in halide perovskites and offer important guidance toward rationally designing more stable and efficient perovskite devices.

Patent
02 Apr 2020
TL;DR: In this paper, the authors provide devices and methods for delivering a biomolecule into a cell, including a first reservoir, a second reservoir, and a porous membrane comprising a nanopore, and two or more electrodes configured to generate an electric field across the porous membrane.
Abstract: The present disclosure provides devices and methods for delivering a biomolecule into a cell. A delivery device of the present disclosure includes a first reservoir, a second reservoir, a porous membrane comprising a nanopore, and two or more electrodes configured to generate an electric field across the porous membrane for delivery of a biomolecule present in the second reservoir through the nanopore of the porous membrane and into a cell present in the first reservoir.

ReportDOI
25 Nov 2020
TL;DR: Yang as discussed by the authors is a S. K. and Angela Chan Distinguished Chair Professor in Energy at the University of California, Berkeley and his main research interests focus on nanoscience for renewable energy conversion and storage.
Abstract: Peidong Yang is S. K. and Angela Chan Distinguished Chair Professor in Energy at the University of California, Berkeley. He is a senior faculty scientist at Materials and Chemical Sciences Division, Lawrence Berkeley National Lab, director for California Research Alliance by BASF and for the Kavli Energy Nanoscience Institute at Berkeley. He is member of both the National Academy of Sciences and the American Academy of Arts and Sciences. He holds B.A. in Chemistry from the University of Science and Technology in China, Ph.D. in Chemistry from Harvard University, and was a postdoc at UC Santa Barbara. His main research interests focus on nanoscience for renewable energy conversion and storage.