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High performance solid-state thermoelectric energy conversion via inorganic metal halide perovskites

Lifu YAN, Lingling ZHAO, Guiting YANG, Shichao LIU, Yang LIU, Shangchao LIN

《能源前沿（英文）》 2022年第16卷第4期页码 581-594 doi: 10.1007/s11708-022-0831-y

摘要： Solid-state thermoelectric energy conversion devices attract broad research interests because of their great promises in waste heat recycling, space power generation, deep water power generation, and temperature control, but the search for essential thermoelectric materials with high performance still remains a great challenge. As an emerging low cost, solution-processed thermoelectric material, inorganic metal halide perovskites CsPb(I_1–xBr_x)₃ under mechanical deformation is systematically investigated using the first-principle calculations and the Boltzmann transport theory. It is demonstrated that halogen mixing and mechanical deformation are efficient methods to tailor electronic structures and charge transport properties in CsPb(I_1–xBr_x)₃ synergistically. Halogen mixing leads to band splitting and anisotropic charge transport due to symmetry-breaking-induced intrinsic strains. Such band splitting reconstructs the band edge and can decrease the charge carrier effective mass, leading to excellent charge transport properties. Mechanical deformation can further push the orbital energies apart from each other in a more controllable manner, surpassing the impact from intrinsic strains. Both anisotropic charge transport properties andZT values are sensitive to the direction and magnitude of strain, showing a wide range of variation from 20% to 400% (with a ZT value of up to 1.85) compared with unstrained cases. The power generation efficiency of the thermoelectric device can reach as high as approximately 12% using mixed halide perovskites under tailored mechanical deformation when the heat-source is at 500 K and the cold side is maintained at 300 K, surpassing the performance of many existing bulk thermoelectric materials.

关键词： inorganic metal halide perovskites mechanical deformation thermoelectrics first-principle calculations Boltzmann transport theory

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Long-lasting photoluminescence quantum yield of cesium lead halide perovskite-type quantum dots

Yonghyun Kim, Huiwen Liu, Yi Liu, Boa Jin, Hao Zhang, Wenjing Tian, Chan Im

《化学科学与工程前沿（英文）》 2021年第15卷第1期页码 187-197 doi: 10.1007/s11705-020-1931-z

摘要： Cesium lead halide perovskite (CsPbX , X= Cl, Br, I) quantum dots (QDs) and their partly Mn -substituted QDs (CsPb Mn X ) attract considerable attention owing to their unique photoluminescence (PL) efficiencies. The two types of QDs, having different PL decay dynamics, needed to be further investigated in a form of aggregates to understand their solid-state-induced exciton dynamics in conjunction with their behaviors upon degradation to achieve practical applications of those promising QDs. However, thus far, these QDs have not been sufficiently investigated to obtain deep insights related to the long-term stability of their PL properties as aggregated solid-states. Therefore, in this study, we comparatively examined CsPbX - and CsPb Mn X -type QDs stocked for>50 d under dark ambient conditions by using excitation wavelength-dependent PL quantum yield and time-resolved PL spectroscopy. These investigations were performed with powder samples in addition to solutions to determine the influence of the inter-QD interaction of the aged QD aggregates on their radiative decays. It turns out that the Mn -substituted QDs exhibited long-lasting PL quantum efficiencies, while the unsubstituted CsPbX -type QDs exhibited a drastic reduction of their PL efficiencies. And the obtained PL traces were clearly sensitive to the sample status. This is discussed with the possible interaction depending on the size and distance of the QD aggregates.

关键词： quantum dots cesium lead halide perovskite time-resolved photoluminescence PL quantum yield QD aggregates

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Formation of secondary inorganic aerosol in a frigid urban atmosphere

《环境科学与工程前沿（英文）》 2022年第16卷第2期 doi: 10.1007/s11783-021-1452-0

摘要：

•Harbin showed relatively high threshold RH (80%) for apparent increase of SOR.

关键词： Haze Sulfate Nitrate Heterogeneous chemistry Biomass burning Northeast China

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Halide-free carbonylation of methanol with H-MOR supported CuCeO

Chaoli Tong, Jiachang Zuo, Danlu Wen, Weikun Chen, Linmin Ye, Youzhu Yuan

《化学科学与工程前沿（英文）》 2021年第15卷第5期页码 1075-1087 doi: 10.1007/s11705-020-2019-5

摘要： Heterogeneous halide-free carbonylation of methanol to acetates, including methyl acetate (MA) and acetic acid, using non-precious metal catalysts has been a topic of interest for decades. The key issue is that the water produced by methanol dehydration inhibits the formation of acetyl species and reduces the MA selectivity. Here, we report that CuCeO /H-mordenite (H-MOR) catalyst can nearly eliminate the inhibiting effect of water on carbonylation by a water-gas shift reaction (WGSR) on-site, and can thus achieve 96.5% methanol conversion with 87.4% MA selectivity for the halide-free carbonylation of methanol. The results of powder X-ray diffraction, transmission electron microscopy, and scanning electron microscopy show that the Cu and Ce species are highly dispersed on H-MOR even when the CuCeO contents are as high as 29 wt-%. Fourier transform infrared spectroscopy and CO chemisorption analysis reveal that a small portion of Cu species can migrate into the channel of H-MOR when CuCeO /H-MOR is calcined at 500 °C and these Cu species are converted into Cu sites upon reduction. The Cu sites facilitate the WGSR and are also active sites for methanol carbonylation. The introduction of Ce benefits the inhibition of coke deposits and thus enhances the catalyst stability.

关键词： methanol carbonylation halide-free methyl acetate H-mordenite copper and cerium oxide

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Reduction of CeO

Elena Yu. KONYSHEVA

《化学科学与工程前沿（英文）》 2013年第7卷第3期页码 249-261 doi: 10.1007/s11705-013-1333-6

摘要： Reduction behavior of pure and doped CeO , the multi-phase La Sr CoO ? CeO , La Sr MnO ? CeO , and La Ni Fe O ? CeO composites, was studied under hydrogen containing atmosphere to address issues related to the improvement of electrochemical and catalytic performance of electrodes in fuel cells. The enhanced reduction of cerium oxide was observed initially at 800°C in all composites in spite of the presence of highly reducible transition metal cations that could lead to the increase in surface concentration of oxygen vacancies and generation of the electron enriched surface. Due to continuous reduction of cerium oxide in La Sr CoO ? CeO and La Sr MnO ? CeO (up to 10 h) composites the redox activity of the Ce /Ce pair could be suppressed and additional measures are required for reversible spontaneous regeneration of Ce . After 3 h exposure to H -Ar at 800°C the reduction of cerium oxides and perovskite phases in La Ni Fe O ? CeO composites was diminished. The extent of cerium oxide involvement in the reduction process varies with time, and depends on its initial deviation from oxygen stoichiometry (that results in the larger lattice parameter and the longer pathway for O transport through the fluorite lattice), chemical origin of transition metal cations in the perovskite, and phase diversity in multi-phase composites.

关键词： reduction of cerium oxide composites perovskites catalyst under hydrogen containing atmosphere

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Spectrokinetics study of probable effects of diverse inorganic ions on bleaching of dye

Rafia AZMAT, Masooda QADRI, Fahim UDDIN

《化学科学与工程前沿（英文）》 2011年第5卷第1期页码 131-138 doi: 10.1007/s11705-010-0556-z

摘要： Toluidine blue (TB) is an important anticoagulant metachromasia molecule showing a pronounced variation in the visible spectrum due to the aggregation phenomenon and electrostatic interaction with the charged synthetic and biologic polymers. The current study describes the interactive role of diverse inorganic material ions on the bleaching of toluidine blue (tolonium chloride) (TB ) with urea in acidic and basic media using the spectrophotometric technique. The spectra of TB and urea with different cations and anions were monitored and their characteristic features are presented here. The negative effect of added cations on reduction may be the result of altered electron pathways which led to suppression of the reduction/bleaching of TB, while a slight decrease in dye reduction by added anions may be due to the scavenging of the OH* radical. It has been observed in the case of Co that in addition to the electron-transfer reaction, other processes like layer and precipitate formation also appear to be taking place. The dye bleaching process followed pseudo first order kinetics with respect to TB, urea, and H ion, whereas significant decoloration in the presence of urea proved that reductants control the redox reaction. No decoloration in acidic medium with diverse ions was seen compared to alkaline media, showing that water pH played an important role in the bleaching of dye. The reduction/bleaching of dye was investigated at different temperatures, and energy parameters were evaluated for a TB -Urea reaction, including the energy of activation ( = 39.60 kJ·mol ), enthalpy of activation (? = 34?kJ·mol ), entropy of activation (? = 146.5 kJ mol ·K ), and free energy of activation (ΔG* = -52.35 kJ·mol ). A mechanism of interaction of diverse ions in dye bleaching and a mechanism of reduction based on the above findings is proposed.

关键词： TB diverse ions suppress decoloration

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Organic and inorganic phosphorus uptake by bacteria in a plug-flow microcosm

Jinbo ZHAO, Xuehua LIU

《环境科学与工程前沿（英文）》 2013年第7卷第2期页码 173-184 doi: 10.1007/s11783-013-0494-3

摘要： Phosphorus (P) is a vital nutrient for sustaining natural water productivity. Both particulate and dissolved forms of organic and inorganic P are potentially important sources of bioavailable P for primary and secondary producers. A microcosm system to imitate the bacterial community in Plym river sediment and pore water is described and bacterial uptake rates for inorganic and organic phosphorus are presented in this paper. The aim of this study was to investigate the uptake of two organic phosphorus compounds (phytic acid and D-glucose-6-phosphate) by freshwater bacteria. The bioreactors comprise glass columns packed with two types of small glass beads on which bacterial biofilm can develop. The glass beads with different porosity were introduced to simulate River SPM. The selected P compounds spiked into the inflow of the microcosm, and measured the step change of P concentration in the outflow to investigate the behavior of bacterial uptake of nutrients. The results showed that organic phosphorus was converted into inorganic phosphorus but the conversion rate depended on the type of phosphorus species. One experiment suggested that phytic acid (refractory) could displace phosphate from the biofilm surface; the other experiment showed that D-glucose-6-phosphate (labile) could be hydrolysed and utilized easily by the bacteria. The results also suggested that bacteria might break down the C-P bonds to utilize the carbon. Further experiments should investigate the effect of varying the C:N:P ratio in the microcosm system to determine which nutrient limits bacteria uptake.

关键词： organic phosphorus bacteria uptake

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氢气分离膜研究进展

栾永超,熊亚林,何广利,刘聪敏,李帅

《中国工程科学》 2022年第24卷第3期页码 140-152 doi: 10.15302/J-SSCAE-2022.03.015

摘要：

氢气是重要的工业原料和清洁燃料，氢气分离具有重要的经济和社会价值；膜分离法装置结构简单、转换高效、投资成本低且环境友好，在氢气分离领域应用前景广阔；氢气分离膜的性能是影响氢气分离过程效率的决定性因素，因而氢气分离膜技术研究一直是国内外膜领域的热点方向。本文阐述了氢气分离膜的应用需求、基本机理，系统梳理了致密金属膜、无机多孔膜、金属‒ 有机框架（MOF）膜、有机聚合物膜、混合基质膜的研究进展。研究发现，尽管无机多孔膜、有机聚合物膜、混合基质膜等具有良好的氢气分离纯化性能，但在分布式、小型化的应用场景下的分离性能仍待改进提高；提高钯基金属膜的抗毒化性能、优化膜的性价比，是促进工业应用的有效手段；整合无机多孔膜、MOF膜的优点，可促进分子筛分机制膜的性能跃升；有机聚合物膜的耐温、机械等性能仍需提高；对现有高分子膜材料进行改性、制备高分子合金，是开发新型气体分离膜的重要方向；混合基质膜在进行可控调节排布后，将显著提高膜性能。多种氢气分离膜的研究和应用，支撑了氢气分离纯化过程的发展，在材料种类丰富、制备工艺进步后将发挥更大的工程价值。

关键词：氢气分离膜；致密金属膜；无机多孔膜；金属‒ 有机框架膜；有机聚合物膜；混合基质膜；氢气纯化

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Immobilization of laccase on organic–inorganic nanocomposites and its application in the removal of phenolic

《化学科学与工程前沿（英文）》 2023年第17卷第7期页码 867-879 doi: 10.1007/s11705-022-2277-5

摘要： Polydopamine-functionalized nanosilica was synthesized using an inexpensive and easily obtainable raw material, mild reaction conditions, and simple operation. Subsequently, a flexible spacer arm was introduced by using dialdehyde starch as a cross-linking agent to bind with laccase. A high loading amount (77.8 mg∙g^‒1) and activity retention (75.5%) could be achieved under the optimum immobilization conditions. Thermodynamic parameters showed that the immobilized laccase had a lower thermal deactivation rate constant and longer half-life. The enhancement of thermodynamic parameters indicated that the immobilized laccase had better thermal stability than free laccase. The residual activity of immobilized laccase remained at about 50.0% after 30 days, which was 4.0 times that of free laccase. Immobilized laccase demonstrated excellent removal of phenolic pollutants (2,4-dichlorophenol, bisphenol A, phenol, and 4-chlorophenol) and perfect reusability with 70% removal efficiency retention for 2,4-dichlorophenol after seven cycles. These results suggested that immobilized laccase possessed great reusability, improved thermal stability, and excellent storage stability. Organic–inorganic nanomaterials have a good application prospect for laccase immobilization, and the immobilized laccase of this work may provide a practical application for the removal of phenolic pollutants.

关键词： polydopamine pollutant removal thermodynamic phenolic pollutants immobilized laccase

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The influence of curing conditions on the mechanical properties and leaching of inorganic polymers made

Remus I. Iacobescu, Valérie Cappuyns, Tinne Geens, Lubica Kriskova, Silviana Onisei, Peter T. Jones, Yiannis Pontikes

《化学科学与工程前沿（英文）》 2017年第11卷第3期页码 317-327 doi: 10.1007/s11705-017-1622-6

摘要： This study reports on the impact of the curing conditions on the mechanical properties and leaching of inorganic polymer (IP) mortars made from a water quenched fayalitic slag. Three similar IP mortars were produced by mixing together slag, aggregate and activating solution, and cured in three different environments for 28 d: a) at 20 °C and relative humidity (RH) ~ 50% (T20RH50), b) at 20 °C and RH≥90% (T20RH90) and c) at 60 °C and RH ~ 20% (T60RH20). Compressive strength (EN 196-1) varied between 19 MPa (T20RH50) and 31 MPa (T20RH90). This was found to be attributed to the cracks formed upon curing. Geochemical modelling and two leaching tests were performed, the EA NEN 7375 tank test, and the BS EN 12457-1 single batch test. Results show that Cu, Ni, Pb, Zn and As leaching occurred even at high pH, which varied between 10 and 11 in the tank test’s leachates and between 12 and 12.5 in the single batch’s leachates. Leaching values obtained were below the requirements for non-shaped materials of Flemish legislation for As, Cu and Ni in the single batch test.

关键词： inorganic polymer geochemical leaching modelling heavy metals recycling non-ferrous fayalitic slag curing

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Enhanced charge extraction for all-inorganic perovskite solar cells by graphene oxide quantum dots modified

《化学科学与工程前沿（英文）》 2023年第17卷第5期页码 516-524 doi: 10.1007/s11705-022-2238-z

摘要： All-inorganic cesium lead bromide (CsPbBr₃) perovskite solar cells have been attracting growing interest due to superior performance stability and low cost. However, low light absorbance and large charge recombination at TiO₂/CsPbBr₃ interface or within CsPbBr₃ film still prevent further performance improvement. Herein, we report devices with high power conversion efficiency (9.16%) by introducing graphene oxide quantum dots (GOQDs) between TiO₂ and perovskite layers. The recombination of interfacial radiation can be effectively restrained due to enhanced charge transfer capability. GOQDs with C-rich active sites can involve in crystallization and fill within the CsPbBr₃ perovskite film as functional semiconductor additives. This work provides a promising strategy to optimize the crystallization process and boost charge extraction at the surface/interface optoelectronic properties of perovskites for high efficient and low-cost solar cells.

关键词： all inorganic perovskite solar cells graphene oxide quantum dots high performance stability

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Thermal transport in organic/inorganic composites

Bin LIU, Lan DONG, Qing XI, Xiangfan XU, Jun ZHOU, Baowen LI

《能源前沿（英文）》 2018年第12卷第1期页码 72-86 doi: 10.1007/s11708-018-0526-6

摘要： Composite materials, which consist of organic and inorganic components, are widely used in various fields because of their excellent mechanical properties, resistance to corrosion, low-cost fabrication, etc. Thermal properties of organic/inorganic composites play a crucial role in some applications such as thermal interface materials for micro-electronic packaging, nano-porous materials for sensor development, thermal insulators for aerospace, and high-performance thermoelectric materials for power generation and refrigeration. In the past few years, many studies have been conducted to reveal the physical mechanism of thermal transport in organic/inorganic composite materials in order to stimulate their practical applications. In this paper, the theoretical and experimental progresses in this field are reviewed. Besides, main factors affecting the thermal conductivity of organic/inorganic composites are discussed, including the intrinsic properties of organic matrix and inorganic fillers, topological structure of composites, loading volume fraction, and the interfacial thermal resistance between fillers and organic matrix.

关键词： thermal conductivity organic/inorganic composites effective medium theory thermal percolation theory interfacial thermal resistance

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Flame-retardant properties of

Kumar Sai SMARAN, Rajashekar BADAM, Raman VEDARAJAN, Noriyoshi MATSUMI

《能源前沿（英文）》 2019年第13卷第1期页码 163-171 doi: 10.1007/s11708-018-0554-2

摘要： This paper focuses on the superiority of organic-inorganic hybrid ion-gel electrolytes for lithium-ion batteries (LiBs) over commercial electrolytes, such as 1 M LiPF in 1:1 ethylene carbonate (EC): dimethyl carbonate (DMC) {1 M LiPF -EC: DMC}, in terms of their flame susceptibility. These ion-gel electrolytes possess ionic liquid monomers, which are confined within the borosilicate or silicate matrices that are ideal for non-flammability. Naked flame tests confirm that the organic-inorganic hybrid electrolytes are less susceptible to flames, and these electrolytes do not suffer from a major loss in terms of weight. In addition, the hybrids are self-extinguishable. Therefore, these hybrids are only oxidized when subjected to a flame unlike other commercial electrolytes used in lithium-ion batteries. Supplementary analyses using differential scanning calorimetric studies reveal that the hybrids are glassy until the temperature reaches more than 100°C. The current results are consistent with previously published data on the organic-inorganic hybrids.

关键词： inorganic polymeric borosilicate network organic-inorganic hybrids self-extinguishability nonflammability lithium batteries flame-retardants

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A comparative study on polypropylene separators coated with different inorganic materials for lithium-ion

Linghui Yu, Jiansong Miao, Yi Jin, Jerry Y.S. Lin

《化学科学与工程前沿（英文）》 2017年第11卷第3期页码 346-352 doi: 10.1007/s11705-017-1648-9

摘要： Coating commercial porous polyolefin separators with inorganic materials can improve the thermal stability of the polyolefin separators and hence improve the safety of lithium-ion batteries. Several different inorganic materials have been studied for the coating. However, there lacks a study on how different inorganic materials affect the properties of separators, in terms of thermal stability and cell performance. Herein, we present such a study on coating a commercial polypropylene separator with four inorganic materials, i.e., Al O , SiO , ZrO and zeolite. All inorganic coatings have improved thermal stability of the separators although with differences. The coating layers add 28%–45% of electrical resistance compared with the pure polypropylene separator, but all the cells prepared with the coated polypropylene separators have the same electrical chemical performance as the uncoated separator in terms of rate capability and capacities at different temperatures.

关键词： lithium-ion battery battery safety composite separator porosity tortuosity

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Mature

Giorgia De Guido, Matteo Compagnoni, Laura A. Pellegrini, Ilenia Rossetti

《化学科学与工程前沿（英文）》 2018年第12卷第2期页码 315-325 doi: 10.1007/s11705-017-1698-z

摘要： Carbon capture and storage (CCS) have acquired an increasing importance in the debate on global warming as a mean to decrease the environmental impact of energy conversion technologies, by capturing the CO produced from the use of fossil fuels in electricity generation and industrial processes. In this respect, post-combustion systems have received great attention as a possible near-term CO capture technology that can be retrofitted to existing power plants. This capture technology is, however, energy-intensive and results in large equipment sizes because of the large volumes of the flue gas to be treated. To cope with the demerits of other CCS technologies, the chemical looping combustion (CLC) process has been recently considered as a solution for CO separation. It is typically referred to as a technology without energy penalty. Indeed, in CLC the fuel and the combustion air are never mixed and the gases from the oxidation of the fuel (i.e., CO and H O) leave the system as a separate stream and can be separated by condensation of H O without any loss of energy. The key issue for the CLC process is to find a suitable oxygen carrier, which provides the fuel with the activated oxygen needed for combustion. The aim of this work is to explore the feasibility of using perovskites as oxygen carriers in CLC and to consider the possible advantages with respect to the scrubbing process with amines, a mature post-combustion technology for CO separation.

关键词： CO₂ capture monoethanolamine chemical looping combustion oxygen carrier perovskites