Atomically Dispersed Nickel(I) on an Alloy-Encapsulated Nitrogen-Doped Carbon Nanotube Array for High-Performance Electrochemical CO 2 Reduction Reaction
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Engineering topics
Publications and source records attributed to Liu, Junfeng.
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Abstract Single‐atom catalysts (SACs) show great promise for electrochemical CO 2 reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single‐atom electrode greatly limit their performance. Herein, we prepared a nickel single‐atom electrode consisting of isolated, high‐density and low‐valent nickel(I) sites anchored on a self‐standing N‐doped carbon nanotube array with nickel–copper alloy encapsulation on a carbon‐fiber paper. The combination of single‐atom nickel(I) sites and self‐standing array structure gives rise to an excellent electrocatalytic CO 2 reduction performance. The introduction of copper tunes the d‐band electron configuration and enhances the adsorption of hydrogen, which impedes the hydrogen evolution reaction. The single‐nickel‐atom electrode exhibits a specific current density of −32.87 mA cm −2 and turnover frequency of 1962 h −1 at a mild overpotential of 620 mV for CO formation with 97 % Faradic efficiency.
Solar reflective cool roofs and walls can be used to mitigate the urban heat island effect. While past research has investigated the climate impacts of adopting cool surfaces, few studies have investigated their effects on air pollution, especially on particulate matter (PM). This study for the first time investigates the influence of widespread deployment of cool walls on urban air pollutant concentrations, and systematically compares cool wall to cool roof effects. Simulations using a coupled meteorology-chemistry model (WRF-Chem) for a representative summertime period show that cool walls and roofs can reduce urban air temperatures, wind speeds, and planetary boundary heights in the Los Angeles Basin. Consequently, increasing wall (roof) albedo by 0.80, an upper bound scenario, leads to maximum daily 8-h average ozone concentration reductions of 0.35 (0.83) ppbv in Los Angeles County. However, cool walls (roofs) increase daily average PM2.5 concentrations by 0.62 (0.85) μg m-3. We investigate the competing processes driving changes in concentrations of speciated PM2.5. Increases in primary PM (elemental carbon and primary organic aerosols) concentrations can be attributed to reductions in ventilation of the Los Angeles Basin. Increases in concentrations of semivolatile species (e.g., nitrate) are mainly driven by increases in gas-to-particle conversion due to reduced atmospheric temperatures.
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Composites incorporating metal nanoparticles (MNPs) within metal-organic frameworks (MOFs) have broad applications in many fields. However, the controlled spatial distribution of the MNPs within MOFs remains a challenge for addressing key issues in catalysis, for example, the efficiency of catalysts due to the limitation of molecular diffusion within MOF channels. We report a facile strategy that enables MNPs to be encapsulated into MOFs with controllable spatial localization by using metal oxide both as support to load MNPs and as a sacrificial template to grow MOFs. This strategy is versatile to a variety of MNPs and MOF crystals. By localizing the encapsulated MNPs closer to the surface of MOFs, the resultant MNPs@MOF composites not only exhibit effective selectivity derived from MOF cavities, but also enhanced catalytic activity due to the spatial regulation of MNPs as close as possible to the MOF surface.
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We present a novel visualization framework—EnsembleGraph— for analyzing ensemble simulation data, in order to help scientists understand behavior similarities between ensemble members over space and time. A graph-based representation is used to visualize individual spatiotemporal regions with similar behaviors, which are extracted by hierarchical clustering algorithms. A user interface with multiple-linked views is provided, which enables users to explore, locate, and compare regions that have similar behaviors between and then users can investigate and analyze the selected regions in detail. The driving application of this paper is the studies on regional emission influences over tropospheric ozone, which is based on ensemble simulations conducted with different anthropogenic emission absences using the MOZART-4 (model of ozone and related tracers, version 4) model. We demonstrate the effectiveness of our method by visualizing the MOZART-4 ensemble simulation data and evaluating the relative regional emission influences on tropospheric ozone concentrations. Positive feedbacks from domain experts and two case studies prove efficiency of our method.