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ACS Sustainable Chemistry & Engineering · 2023 · IF 8.4

One-Step Synthesis of Ammonia Directly from Wet Air/N2 by Plasma Combined with a γ-Al2O3 Catalyst

Jiayu Feng,Ping Ning,Kai Li,Xin Sun,Chi Wang,Lijuan Jia,Maohong Fan

The conventional Haber–Bosch NH3 synthesis process requires high temperatures and pressures, resulting in a high carbon footprint and the need to develop alternative NH3 synthesis methods. Accordingly, plasma-based and γ-Al2O3-catalyzed NH3 synthesis from H2O (a hydrogen source) and air/N2 (a nitrogen source) was studied under low temperature and low pressure conditions. The experimental results show that NH3 can be synthesized with air/N2 and H2O, although byproducts such as NO and N2O are also formed. The NH3 formation rate resulting from the use of N2 and H2O is higher than that of air and H2O. Increasing specific energy input (SEI) can increase the NH3 formation rate. Nevertheless, the energy efficiency of NH3 synthesis technology first increases and then decreases with SEI. An NH3 formation rate of 2.92 μmol h–1 g–1 was achieved with an SEI of 11.68 J mL–1 and energy efficiency of 5.10 mg kW–1 h–1 (1.28 mg kWh–1g–1), when wet air at a flow rate of 200 mL min–1 was introduced into the dielectric barrier discharge (DBD) reactor, which was lower than that (4.30 μmol h–1 g–1) attained with N2 + H2O under an SEI of 11.50 J mL–1 and energy efficiency of 7.63 mg kW–1 h–1 (1.91 mg kWh–1g–1). Additionally, the γ-Al2O3 catalyst exhibited good stability. Different results show that plasma-based and γ-Al2O3 catalyzed NH3 synthesis technology is promising.

CAS / MDL: 1344-28-1
研究领域: 化学工程 · 环境科学 · 催化材料
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ADVANCED FUNCTIONAL MATERIALS · 2024 ·Vol. 34 ·期 30 ·2316036 · IF 18.5

Robust Macroscale Superlubricity in Humid Air via Designing Amorphous DLC/Crystalline TMDs Friction Pair

Dongxiang Zhu,Jie Zhang,Panpan Li,Zhan Li,Hongxuan Li,Xiaohong Liu,Tianbao Ma,Li Ji,Huidi Zhou,Jianmin Chen

Superlubricity, a cutting-edge concept, has the potential to drive the Fourth Industrial Revolution giving its near-zero energy consumption, but the challenge is how to achieve it in humid air with chemical activity and at macroscale surfaces with unavoidable defects. Here, a novel principle involving the amorphous/crystalline  friction pair based on the cognition that tribochemical interaction sites originate from grain boundary defect locations is proposed to achieve macroscale superlubricity in humid air. The absence of grain boundaries in amorphous diamond-like carbon (DLC) significantly reduces chemical interaction during the sliding process. This is supported by experimental observations of priority oxidation at the grain boundaries. Results indicate DLC versus MoS 2 friction pair has weakened chemical interaction and less humid insensitivity compared to the MoS 2 versus MoS 2 pair, even increasing the contact area. Theoretical simulation suggests that DLC versus MoS 2 pair eliminates the cross-linking of friction interlayers induced by the enrichment of H 2 O molecules at MoS 2 defects. The robust superlubricity is achieved for the typical friction pair of DLC versus MoS 2 in air (RH≤25%) at macroscopic contact pressure (1.1 GPa) with friction coefficient in 10 −3 magnitude and extra-long anti-wear life (more than 2 × 10 5 cycles), which is of significance for the industrialization of superlubricity.

CAS / MDL: 12138-09-9
研究领域: 材料科学 · 摩擦学 · 表面工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Energy-efficient removal of trace VOCs from humid air using metal-organic gel derived porous carbon

Sadia Rehman,Xianming Zheng,Pengyi Zhang

The development of granular adsorbents for the efficient capture of low-concentration volatile organic compounds (VOCs) from humid air are highly desirable. Herein, we report the synthesis of granular ZIF-8 monolith ( mono ZIF-8) featuring high surface area (2312 m 2 /g) and mesoporous structure by shortening the synthesis time and optimizing the reactant concentrations, which was further carbonized at 1000 °C to obtain porous granular carbon. As-prepared ZIF-8-C1000 exhibited high surface area (1623 m 2 /g), hierarchical porous structure (0.5–10 nm) and hydrophobicity (water contact angle 145.8°), thus it showed very high adsorption performance for trace VOCs like toluene and hexanal under both dry and humid conditions (relative humidity 30 %-80 %) at 25 °C, much higher than commercial activated carbon (AC) such as BPL-AC, coconut shell AC, and representative MOFs including HKUST-1, mono HKUST-1, mono MIL-100(Fe), MIL-101(Cr) and MOF-235. Additionally, ZIF-8-C1000 could be rapidly regenerated under mild temperatures (60 °C to 80 °C), while BPL-AC requires a higher desorption temperature and more time due to disordered porosity. The exceptional adsorption and desorption performance of granular ZIF-8-C1000 over BPL-AC can be attributed to its interconnected micropores and mesopores.

研究领域: 材料科学 · 环境工程 · 化学工程
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Journal of Cleaner Production · 2024 · IF 9.7

Performance evaluation of a wet air oxidation reactor with external circulation for high-chemical oxygen demand wastewater treatment

Xiemin Liu,Yu Gao,Xinyao Li,Weimin Meng,Feng Zhang,Zhibing Zhang,Zheng Zhou

The presence of high-concentration organic contaminants in wastewater poses considerable risks to the health of both humans and ecosystems. Wet air oxidation (WAO) is an attractive treatment option, but current dilution and retreatment processes do not align with economic and environmental principles. Here we report an external circulation wet oxidation treatment process that utilizes oxidizing liquids to reduce feed concentration. By coupling energy consumption model with computational fluid dynamics model, we explore the optimal parameters for an industrial external circulation reactor. A 90 kt/a external circulation wastewater treatment system has been established, achieving a 21.6% increase in chemical oxygen demand (COD) removal efficiency and a 34.8% reduction in energy consumption. These findings provide a promising pathway for the efficient, low-energy treatment of high-concentration organic wastewater while minimizing freshwater resource consumption.

研究领域: 环境工程 · 化学工程
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ENERGY CONVERSION AND MANAGEMENT · 2022 · IF 11.533

Experimental analysis of a high-performance open sorption thermal storage system with absorption-crystallization-adsorption processes

Abel Mehari,R.Z. Wang,Z.Y. Xu

Sorption thermal energy storage is one of the promising solar thermal energy storage considering its long-term storage ability. Since the common sorption thermal storage suffers from low sorption capacity, a high energy storage density enhancement mechanism is always essential for a cost-effective and compact storage system. With three-phase sorption thermal storage, high energy storage density from the crystallization sorption process can be achieved. However, such a sorption process brings significant challenges, including crystal blockage issues in absorption system or solution leakage handling problems in adsorption system, which need to be resolved. Here, we showed a high-performance sorption thermal storage that can attain high energy storage density via a full liquid-to-solid state sorption process. Such a process is achieved by adopting moist air as heat and mass transfer media, which enables liquid absorption, crystallization, and solid adsorption in a simple configuration simultaneously. The lab-scale model achieved high energy storage density in the range of 333–405 kWh/m 3 resulting from the heat of absorption and crystallization of LiCl, which is the record value for liquid absorption systems. The energy storage density obtained from the dual liquid and solid sorption processes is enhanced by 278 % compared with that of the conventional cycle at 70 % RH (relative humidity) and temperature lift of 10 °C. With simple construction and high energy storage density, the proposed system has great potential in real applications.

CAS / MDL: 7447-41-8
研究领域: 能源技术 · 材料科学
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Pressureless sintering of Al-free Ta-doped lithium garnets Li7-xLa3Zr2-xTaxO12 and the degradation mechanism in humid air

Tianhang Zhang,Timothy Daniel Christopher,Saifang Huang,Yan’gai Liu,Wei Gao,Tilo Sӧhnel,Peng Cao

In this work, pressureless sintering (PLS) method was used to prepare Li 7 La 3 Zr 2 O 12 based Al-free garnet electrolytes with the substitution of tantalum (Ta). A series of Ta-doped lithium garnets Li 7- x La 3 Zr 2- x Ta x O 12 (LLZTO, x  = 0, 0.25, 0.5, 0.75 and 1.0) were prepared, and the effect of Ta on the structure, densification and ionic conductivity was investigated. Both relative density and ionic conductivity of the LLZTO pellets are dependent on the content of Ta substitution, with the maximum values being reached at x  = 0.5. We also studied the stability and degradation mechanism of lithium garnets (Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 ) in humid air with relative humidity of above 70%. It is revealed that after exposure in the humid air for 4 weeks, a layer of LiOH∙H 2 O was observed on the grain boundaries, which lowered its ionic conductivity considerably. In comparison, the pellet stored in a desiccator had clear surface with negligible change in the ionic conductivity.

CAS / MDL: 1312-81-8 1314-23-4
研究领域: 材料科学 · 能源存储与转换
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2021 · IF 3.764

Mechanism of Electrocatalytic Wet Air Oxidation of PPCPs over Solid Catalysts: Kinetic Insight with a Universal Model

Min Sun,Miao-Miao Hou,Xian-Zhang Wang,Bao-Jun Yang,Lin-Feng Zhai,Shaobin Wang

Electrocatalytic wet air oxidation (ECWAO) is a novel wet air oxidation technology using an anodic electric field to stimulate oxygen for catalytic oxidation of water pollutants at ambient condition. Herein, a mechanistic kinetic model is established based on the degradation of bisphenol A in an ECWAO process with manganese oxide (MnOx) catalysts, and the general applicability of the model is verified by triclosan degradation over a Ni@NiO catalyst and sulfamethoxazole degradation over a MnMoOx catalyst. Elementary steps involved in solid-catalyzed reaction and the assistant role of anodic electric field in the catalysis are taken into consideration. A group of kinetic equations based on the Langmuir–Hinshelwood–Hougen–Watson (LHHW) or Eley–Rideal (ER) rate laws are evaluated using the criteria of the minimization of the residual sum of squares and average error. The results show that the ECWAO reaction is best described by the LHHW model in which the surface reaction between adsorbed oxygen and adsorbed organic molecules is the rate-determining step. The key parameters controlling ECWAO reaction kinetics are the adsorption equilibrium constant of oxygen and rate constant of the surface reaction. According to the kinetic model, the reaction rates of organic pollutants are nearly linear dependent upon their concentrations within a certain range. With the increment of the circuit current, the reaction rates of organic pollutants first rise, then reach a plateau, and finally decline. The mechanistic kinetic model proves to be applicable for interpreting and predicting the ECWAO rates of organics over the transition metal oxide catalysts.

研究领域: 环境科学 · 化学工程
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Journal of Energy Chemistry · 2019 · IF 5.162

Li4-xSbxSn1-xS4 solid solutions for air-stable solid electrolytes

Zhuoran Zhang,Jianxing Zhang,Yulong Sun,Huanhuan Jia,Linfeng Peng,Yunyang Zhang,Jia Xie

The sulfide solid electrolytes have the characteristics of high ionic conductivity and low grain boundary resistance, which make them suitable for bulk-type all-solid-state batteries. However, most of them suffer from poor stability in air. Here, we explore the air stable sulfide solid electrolytes in Li 4 SnS 4 -Li 3 SbS 4 system. The solid solutions of Li 4– x Sb x Sn 1– x S 4 (0 ≤  x  ≤ 0.5) can be formed in Li 4 SnS 4 -Li 3 SbS 4 system. Li 3.8 Sb 0.2 Sn 0.8 S 4 achieves the highest ionic conductivity of 3.5 × 10 −4  S cm −1 in this system, which is 5 times as that of Li 4 SnS 4 and 3 orders of magnitude higher than that of Li 3 SbS 4 , respectively. Li 3.8 Sb 0.2 Sn 0.8 S 4 crystallizes into the same structure with high ionic conductivity phase of β -Li 3 PS 4 . Moreover, Li 3.8 Sb 0.2 Sn 0.8 S 4 owns good stability in humid air . Matching with LiCoO 2 and Li 4 Ti 5 O 12 , Li 3.8 Sb 0.2 Sn 0.8 S 4 exhibits the potential to be applied in all-solid-state batteries.

研究领域: 材料科学 · 电化学 · 固体离子学 · 储能技术
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MATERIALS RESEARCH BULLETIN · 2018 · IF 2.873

Electrochemically reduced graphene oxide nanosheet coatings as solid lubricants in humid air

Yongjin Mai,Hongjie Ling,Fuxian Chen,Cansen Liu,Liuyan Zhang,Xiaohua Jie

A facile, low cost and green approach to fabricating graphene nanosheet coatings is reported. It is composed of spraying graphene oxide (GO) suspension to form GO nanosheet coatings followed by a low voltage electrochemical reduction process. The tribological performance of the as-prepared electrochemically reduced graphene oxide (ERGO) nanosheet coatings on copper disk are evaluated by sliding against steel ball in humid air. The friction coefficient of copper is reduced to 1/6 its value, and its specific wear rate is reduced more than two orders of magnitude when copper disk is coated with ERGO nanosheet coatings. These improved tribological performance are attributed to the presence of ERGO nanosheets in the sliding interface of steel vs. copper friction pair. They not only provide easy shearing, reducing the friction coefficient, but also effectively suppress abrasive wear and adhesive wear, decreasing the wear rate of copper disk.

研究领域: 材料科学 · 纳米技术 · 摩擦学
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NEW JOURNAL OF CHEMISTRY · 2023 ·Vol. 47 ·期 41 ·19077-19086 · IF 3.3

Machine-learning-aided identification of ethanol in humid air using zinc complex capped CsPbBr3 resistive sensors

Yue Wang,Xi Wang,Hui Zhang,Shasha Gao,Wenjie Xu,Yulong Zhao,Mingzhi Jiao,Sheng Huang,Xiuquan Gu

In this work, a facile room-temperature (RT) solution-processing strategy was developed to synthesize perovskite CsPbBr3 quantum dots (QDs), which were then modified with Zn-based organic ligands for enhancing their ambient environment and moisture stability. The as-prepared perovskite QDs were well dispersed in a trimethylbenzene solvent with a small particle size of ∼9 nm. Afterwards, a sensor was fabricated by spin-coating perovskite QDs on an interdigital electrode, leading to a sensitivity of 0.025 towards 400 ppm ethanol gas as well as a response/recovery time of 3.9 s/3.6 s at RT. This excellent sensing performance is attributed to the high carrier mobility and adjustable crystal structure of perovskite CsPbBr3 QDs. Theoretical calculation results verified that the sensitivity towards ethanol might result from the formation of chemical bonds between perovskite QDs and Zn-based ligands, leading to a change of molecular orbital energy levels. Furthermore, with a combination of machine-learning algorithms, accurate recognition of ethanol was realized in an ambient environment with high humidity. Our research might be helpful to construct an intelligent sensor for application under complex conditions, such as coal mines and chemical factories.

研究领域: 材料科学 · 化学传感器 · 机器学习
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Energy Storage Materials · 2023 · IF 20.4

High-entropy substitution: A strategy for advanced sodium-ion cathodes with high structural stability and superior mechanical properties

Xing-Yu Du,Yan Meng,Hongyan Yuan,Dan Xiao

O3-type sodium layered oxides are promising energy storage materials because of their high initial Na content and 2D diffusion channels. However, the undesired structural degradations during the repeated charging/discharging process and the severe performance fade following the brief exposure to the humid air, have greatly limited their practical application. Herein, by introducing high-entropy components into the crystal structure of O3-NaNi 0.5 Mn 0.5 O 2 , these concerns are significantly alleviated. To do this, eight metal species sharing the same site are introduced into the transition metal slabs, thus achieving an in-plane high-entropy configuration, which exhibits a postponed phase evolution, an enhanced humid-air stability, and a soothing evolution of interlayer distance. In addition, the stronger mechanical properties of micro-scale particles are also achieved in this multi-component substituted cathode, which keeps the particle integrity even after a long-term cycle. Our work provides an important guidance for the study of high-entropy substitution strategies in the sodium-ion layered cathodes.

研究领域: 储能材料 · 电化学 · 材料科学 · 钠离子电池 · 晶体工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Higher oxygen vacancy content and hydration capability enabled by magnesium doping for high-activity protonic ceramic fuel cell cathode

Liming Zhang,Bingjie Pang,Shiqing Hu,Zhongwei Cao,Peng Zhang,Xuefeng Zhu,Weishen Yang

Protonic ceramic fuel cells (PCFCs) are promising power generation equipment because of their high efficiency and low operating temperature. However, the sluggish oxidation-reduction reaction (ORR) kinetics of the cathode seriously limits their further development. Here, a low-valent alkaline-earth metal Mg-doped BaCo 0.4 Fe 0.4 Zr 0.2 O 3-δ (BaCo 0.4 Fe 0.4 Zr 0.1 Mg 0.1 O 3-δ  = BCFZMg0.1) cathode is developed to increase oxygen vacancy concentration and hydration capability of mixed oxygen ion-electron conducting (MIEC) electrode materials . The phase composition , microstructure, and stability in wet air were examined, while the oxygen vacancy , hydration capability, conductivity, and surface species of the materials were investigated. Experimental results demonstrate that the oxygen vacancy concentration, hydration capability, and conductivity are all increased by Mg doping. Consequently, the ORR active sites were expanded to the whole electrode surface , and the electrochemical performance of PCFCs with BCFZMg0.1 cathode was greatly improved (peak power density: >40% increase; polarization resistance : 60–70% decrease). This work provides a new strategy to develop cathodes with high ORR activity for PCFCs by doping Mg into the MIEC perovskite B-site.

研究领域: 材料科学 · 能源工程 · 电化学
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