Fabrication of Highly Dispersed Ru Catalysts on CeO 2 for Efficient C 3 H 6 Oxidation
Not provided.
Engineering↗
Engineering topics
Jiang, Nan
Publications and source records attributed to Jiang, Nan.
Satellite-Dominated Sulfur L 2,3 X-ray Emission of Alkaline Earth Metal Sulfides
The sulfur L 2,3 X-ray emission spectra of the alkaline earth metal sulfides BeS, MgS, CaS, SrS, and BaS are investigated and compared with spectra calculations based on density functional theory. Very distinct spectral shapes are found for the different compounds. With decreasing electronegativity of the cation, that is, increasing ionic bonding character, the upper valence band width and its relative spectral intensity decrease. These general trends are qualitatively reproduced by the spectra calculations, which give quite an accurate description of the spectral shapes in the upper valence band region. On the low energy side of the sulfur 3s → 2p transition dominating the spectra, we find strong satellites caused by "semi-Auger" decays involving configuration interaction. These satellites, previously believed to be energetically forbidden for sulfur L 2,3 emission and only observed for the L 2,3 emission of Cl to Cr, increase in intensity as the bonding character becomes more ionic and dominate the spectra for SrS and BaS. The intensities, energies, and widths of the satellites vary strongly between the investigated compounds, giving a very specific spectral fingerprint that can be used for speciation analysis.
36 MATERIALS SCIENCE↗
Paired electrocatalysis in 5-hydroxymethylfurfural valorization
5-Hydroxymethylfurfural (HMF) has aroused considerable interest over the past years as an important biomass-derived platform molecule, yielding various value-added products. The conventional HMF conversion requires noble metal catalysts and harsh operating conditions. On the other hand, the electrocatalytic conversion of HMF has been considered as an environmentally benign alternative. However, its practical application is limited by low overall energy efficiency and incomplete conversion. Paired electrolysis and highly efficient electrocatalysts are two viable strategies to address these limitations. Herein, an overview of coupled electrocatalytic HMF hydrogenation or hydrogen evolution reaction (HER) with HMF oxidation as well as the associated electrocatalysts are reviewed and discussed. In this mini-review, a brief introduction of electrocatalytic HMF upgrading is given, followed by the recent advances and challenges of paired electrolysis with an emphasis on the integration HMF electrohydrogenation with HMF electrooxidation. Finally, a perspective for a future sustainable biomass upgrading community based on electrocatalysis is proposed.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Nanophotonics for Chemical Imaging and Spectroscopy
The manipulation of light and light-matter interactions on the nanoscale is enabled by the unique optical properties of plasmonic metal nanostructures and nanoparticles. Indeed, engineered hybrid molecular-plasmonic nanostructures have enabled single molecule detection and identification via surface-enhanced Raman scattering (SERS). Further, the same effect is at the core of visualizing single molecules with sub-nanometer spatial resolution via tip-enhanced Raman scattering (TERS). More generally, modern applications of plasmon-enhanced spectroscopy and microscopy fueled advances in fields as diverse as quantum and semiconductor materials, heterogeneous catalysis, and the health sciences, to name a few. All these exciting developments and many more are touched in this virtual special issue (VSI) on nanophotonics. From ultra-precise chemical imaging measurements performed in a scanning tunneling microscope chamber to single molecule spectroscopic measurements performed at solid-air and solid-liquid interfaces, this VSI includes contributions from active practitioners that are all striving to better-understand increasingly complex interfaces encountered in the biological, materials, and chemical sciences.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Novel and effective surface passivation for high efficiency n- and p-type Silicon solar cell
The project objective was to develop a novel Si surface passivation method using chalcogens, sulfur (S) and/or selenium (Se), as passivating elements, to withstand industry-standard high temperature contacting and metallization schemes for p-type Si based passivated emitter and rear contact (p-PERC) solar cells. The back surface passivation of PERC cells has been improved drastically with the invention and successful application of an Al 2 O 3 passivation layer. However, the front n + diffused junction surface is still poorly passivated by the standard amorphous silicon nitride (SiNx) anti-reflection coating (ARC) layer. This project sought to address the passivation challenges of both front n+ emitter and undiffused p-Si back surface. Improved p-PERC solar cell performance with open circuit voltage (V OC ) > 680 mV and efficiency of 22% were targeted to validate superior defect passivation properties as compared to standard SiO 2 / Al 2 O 3 passivation. During this project, we systematically investigated process-structure-properties-performance relationships of this novel advanced defect passivation approach. The S/Se passivation was carried out by reacting industrial Czochralski (Cz) Si wafers in H 2 S and H 2 Se gases in a chemical vapor deposition (CVD) reactor at temperatures up to 700°C. After an exhaustive optimization of the process parameters (temperature, time, and gas concentration), we established an optimized process and demonstrated extremely low surface recombination velocities (SRVs) of 1.5 cm/s and 8 cm/s on n-type and p-type Si, respectively, by S-passivation. In-depth surface and interface characterization were performed using soft x-ray and photoelectron spectroscopies (XPS, UPS, XES), combined with capacitance-voltage-frequency (C-V-f) measurements, to decipher the surface chemical/electronic structure and interface defect state densities. These measurements provided critical understanding of the defect passivation mechanism and elucidated the presence of surface S-Si bonds, a reduction of surface dipoles, and low interface state densities (D it ) < 10 11 cm -2 ev -1 . We also found that the Se-passivation is inferior to the S-passivation (by at least one order of magnitude in SRV). Application of the optimized S-passivation to the n+ diffused emitter surface led to a low surface recombination current density, J0 ≈ 40 fA/cm 2 (~ 1/4 of the industry-standard SiNx-passivation), and high implied V OC (686 mV) in p-PERC solar cell structures. The S-passivation process also was found to improve the bulk quality of the p-type Si, better than the SiO 2 or Al 2 O 3 passivation processes. After successful demonstration of efficient passivation of Si surface defects by S, we extensively studied the air, thermal, and illumination stability of the passivation structure. S-passivation itself degrades in air due to competing reactions with moisture and oxygen to form oxides, which can be eliminated by a SiNx capping layer (also acting as a anti-reflective coating). After SiNx process optimization, we demonstrated illumination and thermally stable S-passivation with SRV < 5 cm/s and J 0 < 80 fA/cm 2 . These enhancements in Si passivation, incorporated into p-PERC cells, achieved an efficiency of 19.93% with V OC = 649 mV, using manufacturing metallization and contacting schemes. The low cell performance (cell V OC is much less than the implied V OC = 686 mV, anticipated from surface passivation) was identified due to degradation of S-passivation during the metal firing step (out-diffusion of S from the Si interface to the SiNx surface). The S-passivation of Si surfaces shows significant promise with excellent passivation quality, essential for high performance (high V OC , high efficiency) solar cells. Integration of this innovative defect passivation into devices, however, demands further development of the capping layer, low temperature (<700°C) metallization process, and/or engineering of advanced device structures. Surface passivation-dominated advanced Si solar cells, such as tunnel oxide passivated contacts and Si heterojunctions, are increasingly of interest due to their high-performance potential and will have a growing photovoltaic market share in the near future.
14 SOLAR ENERGY↗
Reconfigurable perovskite nickelate electronics for artificial intelligence
Reconfigurable devices offer the ability to program electronic circuits on demand. Here, in this work, we demonstrated on-demand creation of artificial neurons, synapses, and memory capacitors in post-fabricated perovskite NdNiO 3 devices that can be simply reconfigured for a specific purpose by single-shot electric pulses. The sensitivity of electronic properties of perovskite nickelates to the local distribution of hydrogen ions enabled these results. With experimental data from our memory capacitors, simulation results of a reservoir computing framework showed excellent performance for tasks such as digit recognition and classification of electrocardiogram heartbeat activity. Using our reconfigurable artificial neurons and synapses, simulated dynamic networks outperformed static networks for incremental learning scenarios. The ability to fashion the building blocks of brain-inspired computers on demand opens up new directions in adaptive networks.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Impact of n -Butylammonium Bromide on the Chemical and Electronic Structure of Double-Cation Perovskite Thin Films
2D/3D perovskite heterostructures have emerged as a promising material composition to reduce nonradiative recombination in perovskite-based LEDs and solar cells. Such heterostructures can be created by a surface treatment with large organic cations, for example, n-butylammonium bromide (BABr). To understand the impact of the BABr surface treatment on the double-cation (Cs 0.17 FA 0.83 Pb(I 0.6 Br 0.4 ) 3 ) (FA = formamidinium) perovskite thin film and further optimize the corresponding structures, an in-depth understanding of the chemical and electronic properties of the involved surfaces, interfaces, and bulk is required. We study the impact of the BABr treatment with a combination of surface-sensitive X-ray photoelectron spectroscopy and bulk-sensitive resonant inelastic soft X-ray scattering (RIXS). A quantitative analysis of the BABr-treated perovskite thin film shows a modified chemical perovskite surface environment of carbon, nitrogen, bromine, iodine, and lead, indicating that the treatment leads to a perovskite surface with a modified composition and bonding structure. With K-edge RIXS, the local environment at the nitrogen and carbon atoms is probed, allowing us to identify the presence of BABr in the perovskite bulk albeit with a modified bonding environment. This, in turn, identifies a "hidden parameter" for the optimization of the BABr treatment and overall performance of 2D/3D perovskite solar cell absorbers.
2D/3D perovskite heterostructure↗
Efficient passivation of n-type and p-type silicon surface defects by hydrogen sulfide gas reaction
An efficient surface defect passivation is observed by reacting clean Si in a dilute hydrogen sulfide-argon gas mixture (< 5% H2S in Ar) for both n-type and p-type Si wafers with planar and textured surfaces. Surface recombination velocities of 1.5 and 8 cm/s are achieved on n-type and p-type Si wafers, respectively, at an optimum reaction temperature of 550oC that are comparable to the best surface passivation quality used in high efficiency Si solar cells. Surface chemical analysis using x-ray photoelectron spectroscopy shows that sulfur is primarily bonded in a sulfide environment, and synchrotron-based soft x-ray emission spectroscopy of the adsorbed sulfur atoms suggests the formation of S-Si bonds. Furthermore, the sulfur surface passivation layer is unstable in air, attributed to surface oxide formation and a simultaneous decrease of sulfide bonds. However, the passivation can be stabilized by a low-temperature (300oC) deposited amorphous silicon nitride (a-Si:NX:H) capping layer.
14 SOLAR ENERGY↗
Sulfate Speciation Analysis Using Soft X-ray Emission Spectroscopy
It is reported that the chemical and electronic structures of 15 different sulfates are studied using S L 2,3 soft X-ray emission spectroscopy (XES). Sulfur L 2,3 XES spectra of sulfates are distinctively different from those of other sulfur compounds, which makes XES a powerful technique for sulfate detection. Furthermore, subtle but distinct differences between the spectra of sulfates with different cations are observed, which allow a further differentiation of the specific compound. Most prominently, the position and width of the emission from "S 3s" derived bands systematically vary for different compounds, which can be understood with electronic structure and spectral calculations based on density functional theory.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Experimental Investigation of Transition to Turbulence as Affected by Passing Wakes: Effects of High FSTI and Increased Rod Spacing
Experimental results from a study of the effects of passing wakes upon laminar-to-turbulent transition in a low-pressure turbine passage are presented. The test section geometry is designed to simulate the effects of unsteady wakes resulting from rotor-stator interaction upon laminar-to-turbulent transition in turbine blade boundary layers and separated flow regions over suction surfaces. Single-wire, thermal anemometry techniques are used to measure time-resolved and phase-averaged, wall-normal profiles of velocity, turbulence intensity and intermittency at multiple streamwise locations over the turbine airfoil suction surface. The Reynolds number based on suction surface length and stage exit velocity is 50,000. This study compares a previously documented base case flow having an approach flow turbulence intensity of 2.5 percent and a wake passing Strouhal number of 0.792 to two additional cases: one having an increased rod spacing case having a wake passing Strouhal number of 0.396, and another having an elevated approach flow turbulence intensity of 10 percent. From these data, the effects of increased rod spacing and elevated FSTI upon transition and separation processes in the near-wall flow are documented. The results show that a decreased wake passing Strouhal number results in an earlier separation with a larger separation bubble, while the elevated FSTI results in earlier separation, but with a shorter, thinner, separation bubble. The data and animations are included in an accompanying CD ROM.
Kaszeta, Richard W.↗
Experimental Investigation of Transition to Turbulence as Affected by Passing Wakes: Effects of High FSTI and Increased Rod Spacing. Animations and Data Files
No abstract available
Kaszeta, Richard W.↗
Heat Transfer and Fluid Dynamics Measurements in the Expansion Space of a Stirling Cycle Engine
The heater (or acceptor) of a Stirling engine, where most of the thermal energy is accepted into the engine by heat transfer, is the hottest part of the engine. Almost as hot is the adjacent expansion space of the engine. In the expansion space, the flow is oscillatory, impinging on a two-dimensional concavely-curved surface. Knowing the heat transfer on the inside surface of the engine head is critical to the engine design for efficiency and reliability. However, the flow in this region is not well understood and support is required to develop the CFD codes needed to design modern Stirling engines of high efficiency and power output. The present project is to experimentally investigate the flow and heat transfer in the heater head region. Flow fields and heat transfer coefficients are measured to characterize the oscillatory flow as well as to supply experimental validation for the CFD Stirling engine design codes. Presented also is a discussion of how these results might be used for heater head and acceptor region design calculations.
Jiang, Nan↗