1. |
- An, Xiaoqiang, et al.
(author)
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Sodium-Directed Photon-Induced Assembly Strategy for Preparing Multisite Catalysts with High Atomic Utilization Efficiency
- 2023
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In: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 145:3, s. 1759-1768
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Journal article (peer-reviewed)abstract
- Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO2 substrate. Na+ was employed as the crucial cement to direct Au single atoms onto TiO2, while the light-induced electron transfer from excited TiO2 to Au(Na+) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO2. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h(-1) that exceeded other Au/TiO2-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.
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2. |
- Cao, Qi, et al.
(author)
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N-Type Conductive Small Molecule Assisted 23.5% Efficient Inverted Perovskite Solar Cells
- 2022
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In: Advanced Energy Materials. - : John Wiley & Sons. - 1614-6832 .- 1614-6840. ; 12:34
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Journal article (peer-reviewed)abstract
- Because of the compatibility with tandem devices and the ability to be manufactured at low temperatures, inverted perovskite solar cells have generated far-ranging interest for potential commercial applications. However, their efficiency remains inadequate owing to various traps in the perovskite film and the restricted hole blocking ability of the electron transport layer. Thus, in this work, a wide-bandgap n-type semiconductor, 4,6-bis(3,5-di(pyridin-4-yl)phenyl)-2-phenylpyrimidine (B4PyPPM), to modify a perovskite film via an anti-solvent method is introduced. The nitrogen sites of pyrimidine and pyridine rings in B4PyPPM exhibit strong interactions with the undercoordinated lead ions in the perovskite material. These interactions can reduce the trap state densities and inhibit nonradiative recombination of the perovskite bulk. Moreover, B4PyPPM can partially aggregate on the perovskite surface, leading to an improvement in the hole-blocking ability at its interface. This modification can also increase the built-in potential and upshift the Fermi level of the modified perovskite film, promoting electron extraction to the electron transport layer. The champion device achieves a high efficiency of 23.51%. Meantime, the sealed device retains approximate to 80% of its initial performance under a maximum power point tracking for nearly 2400 h, demonstrating an excellent operational stability.
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3. |
- Chen, Xiaochang, et al.
(author)
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Automatic Overtaking on Two-way Roads with Vehicle Interactions Based on Proximal Policy Optimization
- 2021
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In: 2021 32nd IEEE Intelligent Vehicles Symposium (IV). - : Institute of Electrical and Electronics Engineers (IEEE). ; , s. 1057-1064
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Conference paper (peer-reviewed)abstract
- Overtaking the lead vehicle on two-way roads in the presence of several oncoming vehicles is a complex task for autonomous vehicles. In this paper, we formulate the overtaking behavior of an ego vehicle based on a deep reinforcement learning (DRL) method. First, a two-way urban road is created, wherein the ego vehicle aims to reach the destination safely and efficiently while considering multiple traffic participants. We use different intelligent driver model (IDM) parameters to account for different drivers' habits. Furthermore, we introduce different responses of other vehicles when the ego vehicle takes overtaking maneuver. Then, a hierarchical control framework is proposed to manage vehicles on the road, which supervises vehicle behaviors at the high layer and controls the motion at the lower layer. The DRL method named Proximal Policy Optimization is applied to derive the high-level decision-making policies. A self-attention mechanism is further introduced to improve the performance of our algorithm. Finally, the overtaking maneuvers of the ego vehicle in different training timesteps are analyzed and how the responses of other vehicles affect the ego one's overtaking behavior is investigated. Simulation results show that our approach can achieve good performance to deal with the two-way road autonomous overtaking task. Supplementary video is available at https://youtu.be/jPEGjM7cBuk.
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4. |
- Chen, Xiao, et al.
(author)
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The association between cumulative cadmium intake and osteoporosis and risk of fracture in a Chinese population
- 2019
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In: Journal of Exposure Science and Environmental Epidemiology. - : Springer. - 1559-0631 .- 1559-064X. ; 29:3, s. 435-443
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Journal article (peer-reviewed)abstract
- Bone is one of the target organs for cadmium toxicity. However, few studies have shown the association between cumulative cadmium intake and prevalence of osteoporosis and bone fracture. In the present study, we evaluated the association between cumulative cadmium intake and osteoporosis and risk of fracture in a Chinese population. A total of 790 subjects (488 women and 302 men) living in a control area and two cadmium-polluted areas were included. The cumulative cadmium intake was estimated by a food survey. The bone mineral density was determined by using single-photon absorptiometry. The cumulative cadmium intakes were 0.48, 2.14, and 11.00 g for men, and 0.42, 2.11, and 11.12 g in women in control, and moderately and heavily polluted areas, respectively. In women, the odds ratios (ORs) of subjects with a cadmium intake between 2.21 and 10.63 g and >10.63 g were 1.30 (95% CI: 0.58-2.94) and 2.36 (95% CI: 1.14-5.16), compared with those with a cadmium intake < 0.58 g after adjusting to the confounders for osteoporosis. The ORs of subjects with a cadmium intake >10.63 g were 2.34 (95% CI: 1.23-4.38) for all of the women and 2.62 (95% CI: 1.02-5.58) in women ≥ 60 years old, compared with those with a cadmium intake <10.63 g after adjusting to the confounders for bone fractures. In men, similar trends were observed, but no statistical significance was found. In addition, those subjects with renal tubular dysfunction showed high risk of bone fracture. Our results indicate that a high level of cumulative cadmium intake is associated with an increased rate of osteoporosis and fractures among women.
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5. |
- Chen, Xiao, et al.
(author)
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The association between dietary cadmium exposure and renal dysfunction - the benchmark dose estimation of reference levels : the ChinaCad study
- 2018
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In: Journal of Applied Toxicology. - : John Wiley & Sons. - 0260-437X .- 1099-1263. ; 38:10, s. 1365-1373
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Journal article (peer-reviewed)abstract
- The tolerable dietary intake of cadmium was recommended at provisional tolerable monthly intake of 25gkg(-1) body weight. However, several studies indicated that this tolerable level should be re-evaluated for sufficient health protection. In this study, we show the reference levels of dietary cadmium intake for renal dysfunction by using a benchmark dose (BMD) approach. A total of 790 subjects (302 men and 488 women) living in control and cadmium-polluted areas were included. The dietary cadmium intake was estimated by a food survey. Blood cadmium, urinary cadmium and renal function markers (microalbuminuria, N-acetyl--d-glucosaminidase [NAG] and its isoform B [NAGB], (2)-microglobulin and retinol binding protein) in urine were measured. We calculated the 95% lower confidence bounds of BMD (BMDLs) of cumulative cadmium intake. In control and two polluted areas, the median cumulative cadmium intake was 0.5, 2.1 and 11.1g. The odds ratio of the intermediate (1.0-3.0g), second highest (3.0-11.0g) and the highest cumulative cadmium intake (>11.0g) compared with the lowest cumulative cadmium intake (<1.0g) were 2.8 (95% CI: 1.4-5.8), 8.1 (95% CI: 3.8-17.2) and 11.4 (95% CI: 6.5-26.4) for urinary NAG and 6.6 (95% CI: 3.2-13.8), 14.8 (95% CI: 6.8-32.2) and 22.5 (95% CI: 10.7-47.5) for urinary NAGB. The BMDLs of cumulative cadmium intake were 1.1-1.2g (benchmark response [BMR]=5%) for urinary NAG, and were 0.7-0.9g (BMR=5%) for urinary NAGB, and were 1.3-1.4g (BMR=5%) for urinary (2)-microglobulin. The BMDLs of cumulative cadmium intake in a Chinese population were lower than the critical standard previously reported. Further evaluations are needed for sufficient health protection. Several studies indicated that the tolerable dietary intake of cadmium should be re-evaluated for sufficient health protection. In this study, we show the reference levels of dietary cadmium intake for renal dysfunction by using benchmark dose (BMD) approach. The lowest BMD lower bound confidence limits of cumulative cadmium intake were 0.7-0.9g (benchmark response=5%). The BMD lower bound confidence limits of cumulative cadmium intake were lower than the critical standard previously reported. Further evaluations are needed for sufficient health protection.
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6. |
- Chen, Xiao, et al.
(author)
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The association between renal tubular dysfunction and zinc level in a Chinese population environmentally exposed to cadmium
- 2018
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In: Biological Trace Element Research. - : Humana Press. - 0163-4984 .- 1559-0720. ; 186:1, s. 114-121
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Journal article (peer-reviewed)abstract
- Microglobulin (UBMG) were measured. The median UCd, BCd, SZn, and HZn were 2.8 and 13.6 μg/g cr, 1.3 and 12.2 μg/L, 1.31 and 1.12 mg/L, and 0.14 and 0.12 mg/g in subjects living in control and polluted areas. The UBMG level of subjects living in the polluted area was significantly higher than that of the control (0.27 vs 0.11 mg/g cr, p < 0.01). SZn, HZn, and Zn/Cd ratios were negatively correlated with UBMG (p < 0.05 or 0.01). Subjects with high SZn concentrations (≥ 1.62 mg/L) had reduced risks of elevated UBMG [(odds ratio (OR) = 0.26, 95% confidence interval (CI) 0.07-0.99)] after controlling for multiple covariates compared with those with lower zinc levels. A similar result was observed in subjects with high HZn (OR = 0.09, 95% CI 0.02-0.48). The ORs of the second, third, and fourth quartiles of Zn/Cd ratio were 0.40 (95% CI 0.19-0.84), 0.14 (95% CI 0.06-0.37), and 0.01 (95% CI 0.02-0.18) for renal dysfunction compared with those of the first quartile, respectively. For those subjects with high level of UCd, high level of SZn and HZn also had reduced risks of elevated UBMG. The results of the present study show that high zinc body burden is associated with a decrease risk of renal tubular dysfunction induced by cadmium. Zinc nutritional status should be considered in evaluating cadmium-induced renal damage.
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7. |
- Chikina, Alla, et al.
(author)
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Band-Order Anomaly at the gamma-Al2O3/SrTiO3 Interface Drives the Electron-Mobility Boost
- 2021
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In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:3, s. 4347-4356
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Journal article (peer-reviewed)abstract
- The rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about 2 orders of magnitude has been demonstrated at the spinel-perovskite gamma-Al2O3/SrTiO3 interface compared to the paradigm perovskite-perovskite LaAlO3/SrTiO3 interface. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in gamma-Al2O3/SrTiO3 which depopulates electron states in the top SrTiO3 layer. This rearrangement of the mobile electron system pushes the electron density away from the interface, which reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel gamma-Al2O3 and perovskite SrTiO3. Band-order engineering, exploiting the fundamental symmetry properties, emerges as another route to boost the performance of oxide devices.
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8. |
- Parbey, Joseph, et al.
(author)
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Progress in the use of electrospun nanofiber electrodes for solid oxide fuel cells : A review
- 2019
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In: Reviews in Chemical Engineering. - : Walter de Gruyter GmbH. - 2191-0235 .- 0167-8299. ; 36:8, s. 879-931
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Journal article (peer-reviewed)abstract
- The application of one-dimensional nanofibers in the fabrication of an electrode greatly improves the performance of solid oxide fuel cells (SOFCs) due to its advantages on electron transfer and mass transport. Various mixed ionic-electronic conducting materials with perovskites and Ruddlesden-Popper-type metal oxide structures are successfully electrospun into nanofibers in recent years mostly in solvent solution and some in melt forms, which are used as anode and cathode electrodes for SOFCs. This paper presents a comprehensive review of the structure, electrochemical performance, and development of anode and cathode nanofiber electrodes including processing, structure, and property characterization. The focuses are first on the precursor, applied voltage, and polymer in the material electrospinning process, the performance of the fiber, potential limitation and drawbacks, and factors affecting fiber morphology, and sintering temperature for impurity-free fibers. Information on relevant methodologies for cell fabrication and stability issues, polarization resistances, area specific resistance, conductivity, and power densities are summarized in the paper, and technology limitations, research challenges, and future trends are also discussed. The concluded information benefits improvement of the material properties and optimization of microstructure of the electrodes for SOFCs.
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9. |
- Wang, Xiaoqiang, et al.
(author)
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Microalgal biomethane production integrated with an existing biogas plant : A case study in Sweden
- 2013
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In: Applied Energy. - : Elsevier BV. - 0306-2619 .- 1872-9118. ; 112:SI, s. 478-484
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Journal article (peer-reviewed)abstract
- Microalgae are considered as potential sources for biodiesel production due to the higher growth rate than terrestrial plants. However, the large-scale application of algal biodiesel would be limited by the downstream cost of lipid extraction and the availability of water, CO2 and nutrients. A possible solution is to integrate algae cultivation with existing biogas plant, where algae can be cultivated using the discharges of CO2 and digestate as nutrient input, and then the attained biomass can be converted directly to biomethane by existing infrastructures. This integrated system is investigated and evaluated in this study. Algae are cultivated in a photobioreactor in a greenhouse, and two cultivation options (greenhouse with and without heating) are included. Life cycle assessment of the system was conducted, showing that algal biomethane production without greenhouse heating would have a net energy ratio of 1.54, which is slightly lower than that (1.78) of biomethane from ley crop. However, land requirement of the latter is approximately 68 times that of the former, because the area productivity of algae could reach at about 400t/ha (dry basis) in half a year, while the annual productivity of ley crop is only about 5.8t/ha. For the case of Växtkraft biogas plant in Västerås, Sweden, the integrated system has the potential to increase the annual biomethane output by 9.4%. This new process is very simple, which might have potential for scale-up and commercial application of algal bioenergy.
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10. |
- Wang, Xiaoqiang, et al.
(author)
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Microalgal Biomethane Production Integrated with an Existing Biogas Plant: A Case Study in Sweden
- 2012
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Conference paper (peer-reviewed)abstract
- Microalgae are considered as potential sources for biodiesel production due to the higher growth rate than terrestrial plants. However, the large-scale application of algal biodiesel would be limited by the downstream cost of lipid extraction and the availability of water, CO2 and nutrients. A possible solution is to integrate algae cultivation with existing biogas plant, where algae can be cultivated using the discharges of CO2 and digestate as nutrient input, and then the attained biomass can be converted directly to biomethane by existing infrastructures. This integrated system is investigated and evaluated in this study. Algae are cultivated in a photobioreactor in a greenhouse, and two cultivation options (greenhouse with and without heating) are included. Life cycle assessment of the system was conducted, showing that algal biomethane production without greenhouse heating would have a net energy ratio of 1.54, which is slightly lower than that (1.78) of biomethane from ley crop. However, land requirement of the latter is approximately 68 times that of the former, because the area productivity of algae could reach at about 400 t/ha (dry basis) in half a year, while the annual productivity of ley crop is only about 5.8 t/ha. For the case of Växtkraft biogas plant in Västerås, Sweden, the integrated system has the potential to increase the annual biomethane output by 9.4 %. This new process is very simple, which might have potential for scale-up and commercial application of algal bioenergy.
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