Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 8
·2370-2379
·
IF 7
Yanli Ruan,Hang Xu,Haikuo Lei,Wenjuan Xue,Tianyu Wang,Shidong Song,Yangyang Yu,Gui-Rong Zhang,Donghai Mei
Zn–air batteries (ZABs) have been widely studied due to their high theoretical energy density, low cost, and high safety. However, the lack of efficient bifunctional electrocatalysts toward both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) hinders their large-scale application. Herein, a dendritic NiS2@Co–N–C/CNF nanoarchitecture is proposed, which was fabricated by high-temperature carbonization of Co-MOFs and a subsequent simple hydrothermal composite method using NiS2 nanosheets. The catalyst is reasonably designed to integrate the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) active sites on the surface of carbon nanofibers. Through the synergy between NiS2 and Co–N–C/CNF and the unique branch–leaf porous structure, the catalyst showed excellent catalytic activity and stability. In an alkaline electrolyte, the OER overpotential of NiS2@Co–N–C/CNF is 300 mV at 10 mA cm−2. The ORR half-wave potential (E1/2) of NiS2@Co–N–C/CNF is 0.8 V. In addition, the superior catalytic activity of NiS2@Co–N–C/CNF could be transferred to a ZAB, which exhibits a maximum peak power density of 181 mW cm−2 along with an ultra-long cycling stability for 1050 and 600 h at discharging current densities of 5 and 10 mA cm−2, respectively. The performance is significantly higher than that of commercial precious metal Pt/C + IrO2 mixed catalysts. The peak power density of solid state ZAB (SSZAB) integrated with NiS2@Co–N–C/CNF is 76 mW cm−2, and it can still maintain excellent cycling stability under different bending states. More impressively, four in-series SSZABs (NiS2@Co–N–C/CNFs) can charge smartphones, indicating their potential feasibility in the field of wearable electronics.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yiyun Zhang,Jianchun Jiang,Jiang Wu,Mengyuan Wen,Jia Wang
Chemical upcycling of waste polycarbonate (PC) into jet fuels through catalytic tandem hydropyrolysis/hydrodeoxygenation (THH) is a practical strategy to generate value from polymer wastes. A process which combining hydropyrolysis with vapor phase hydrodeoxygenation (HDO) was proposed in a two-stage pressurized fixed-bed reactor. A cobalt-based Metal-Organic Framework (MOF) derived material supported with nickel was designed for the vapor-phase HDO of phenolic compounds derived from PC hydropyrolysis. The product distribution could be regulated by optimizing reaction pressure in the reactor and catalyst to PC mass ratio. Experimental results showed that the products are all phenolic compounds in the absence of catalysts, while a high yield of jet-fuel range cycloalkanes (100%) was obtained under optimized conditions (7 bar H 2 pressure and 5:1 catalyst to PC mass ratio) over NiCo/C. The high HDO activity of NiCo/C depends on the synergistic effect of nickel and cobalt atoms, which facilitates the elimination of phenolic hydroxyl group and hydrogenation of benzene ring . This work puts forward an efficient approach for upcycling PC waste into jet fuels with MOF-derived NiCo/C as a catalyst.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Shuyue Pang,Yanhong Li,Xiaofang Chen,Aisheng Huang
The fabrication of mixed matrix membranes (MMMs) by intermixing suitable fillers with organic polymers is an effective strategy to surmount the well-known trade-off effect between gas permeability and selectivity, which can promote separation performance of membranes to a great extent. Two-dimensional (2D) metal-organic frameworks (MOFs) are considered as potential fillers for strengthening the separation performance of MMMs as they possess high aspect ratio and distinctive chemical characteristics. However, it remains challenging in engineering the morphology of the MOFs with desired pore structure and high aspect ratio. In this study, we firstly prepare c-axis oriented ZIF-95 sheets with lateral dimension exceeding 22 μm and thickness of around 3 μm by the solvothermal method. And then the ZIF-95 sheets are incorporated into the polyimide (PI) matrix to fabricate highly c -axis oriented ZIF-95@PI MMMs (denoted as COZIF-95@PI MMMs thereafter). Attributing to the straight permeation channel of ZIF-95 (3.6 Å) for gas permeation as well as its high compatibility with polyimide substrates, the COZIF-95@PI MMMs show a high gas separation capability. At 373 K and 100 kPa for the COZIF-95@PI MMM with 40 wt% loading, the mixture separation factors of H 2 /CH 4 and H 2 /CO 2 are 134 and 58, respectively, and the H 2 permeability exceeds 967 barrer , which is hopeful for the separation and purification of hydrogen.
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RSC Advances
·
2023
·Vol. 13
·期 23
·15934-15941
·
IF 3.9
Xiaoping Chen,Xianfei Wang,Wei Liu,Hui Tian,Yupeng Du,Haisheng Wei,Linsheng Tang
1-Butene, as one of the widely used chemical raw materials, can be produced by the double bond isomerization of 2-butene. However, the current yield of the isomerization reaction is only up to 20% or so. It is therefore an urgent issue to develop novel catalysts with higher performances. In this work, a high-activity ZrO2@C catalyst that is derived from UiO-66(Zr) is fabricated. The catalyst is prepared by calcining the precursor UiO-66(Zr) at high temperature in nitrogen, and characterized by XRD, TG, BET, SEM/TEM, XPS and NH3-TPD. The results demonstrate that the calcination temperature has significant influences on the catalyst structure and performance. Regarding the catalyst ZrO2@C-500, the selectivity and yield of 1-butene are 94.0% and 35.1%, respectively. The high performance is due to multiple aspects, including the inherited octahedral morphology from parent UiO-66(Zr), suitable medium-strong acidic active sites and high surface area. The present work will lead to a better understanding of the ZrO2@C catalyst and guide the rational design of high-activity catalysts for the double bond isomerization of 2-butene to 1-butene.
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PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Ziyu Jia,Jun Hu,Ping Lu,Yahui Sun,Yunjun Wang
Herein, using Ru/C and H 2 WO 4 as the catalysts, native lignin in biomass was efficiently depolymerized into monophenols following the lignin-first strategy at mild conditions. Upon the co-presence of Ru/C and H 2 WO 4 , birch lignin afforded monophenols in 40.4 wt% yield at 200 °C, which was 2.5 times that upon Ru/C and 7.5 times that upon H 2 WO 4 . 4-Propylsyringol and 4-propylguaiacol were two major products with a combined selectivity of 73%. 2D HSQC NMR of liquid product reveals that β-O-4 bonds in the soluble lignin fragments had been thoroughly disrupted. H 2 WO 4 dissolving at high temperatures promoted the solvolysis of lignin from the biomass matrix, and Ru/C enhanced the following reductive depolymerization. The solid catalysts can be readily recovered for reuse at room temperature after the hydrolysis of carbohydrates, and the catalysts exhibited high activity after four recycles.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Huying Yan,Yang Guo,Xingzhi Bai,Jiawei Qi,Xiangyu Zhao,Haipeng Lu,Longjiang Deng
Developing a lightweight microwave absorbing materials (MAMs) with high absorption capacity at low thickness is a perennial challenge in materials engineering. Herein, a light Ti 3 C 2 T x @Carbon/NiZn ferrite (Ti 3 C 2 T x @C/NZFO) composite is designed by synergistically incorporating dielectric–magnetic components. The inclusion of C and NZFO enhances the interfacial polarization of the substrate and optimizes its impedance matching. Additionally, the presence of NZFO also produces magnetic loss mechanisms, such as natural and exchange resonance, as well as eddy current loss. Spontaneously, Ti 3 C 2 T x @C/NZFO composite achieved a minimum reflection loss ( RL ) of –44.7 dB at 12.5 GHz and displayed an effective absorption bandwidth of 4.27 GHz (13.53–17.8 GHz) at a thin thickness of 1.3 mm ( RL < –10 dB). Besides, the Ti 3 C 2 T x @C/NZFO composite exhibits the smallest radar cross–section (RCS) value, which further corroborates its outstanding microwave absorption performance. This research offers a groundbreaking approach to designing lightweight and thin MAMs.
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Metals
·
2023
·Vol. 13
·期 5
·937
·
IF 2.9
Chuanbin Wang,Yongxin Cheng,Sumeng Hu,Kejia Kang,Yuzhe Han,Xudan Zhang,Ronghan Wei,Guoqiang Luo
W-Si-C composites with high relative densities and good mechanical and wear properties were successfully prepared by spark plasma sintering. The influence of SiC content on the relative density, microstructure, mechanical properties and wear characteristics was investigated. The results indicated that the reaction between SiC and W at their interface produced W2C and W5Si3. SiC also reacted with oxygen impurities at the W grain boundary to form SiO2. The purification of the grain boundaries of W was carried out by SiO2synthesis. Reactive sintering reduces the free energy of the system and facilitates the densification process of W-Si-C composites. This results in a significant increase in the relative density of W-Si-C composites, which reaches a maximum of 98.12%, higher than the 94.32% of pure tungsten. The hardness significantly increases from 4.33 GPa to 8.40 GPa when the SiC content is 2 wt% compared to pure tungsten due to the generation of the hard ceramic phase and the increase in relative density. The wear resistance of the W-Si-C composites was significantly improved with little SiC addition. The wear rate significantly decreased from 313.27 × 10−3mm3/N·m of pure tungsten to 5.71 × 10−3mm3/N·m of W-0.5 wt% SiC. SEM analyses revealed that the dominant wear mechanism of pure tungsten was attributed to fatigue wear, while that of W-Si-C composites was due to abrasive wear.Keywords:W-Si-C composites;spark plasma sintering;interface reaction;mechanical properties;wear characteristics
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高影响因子
FUEL
·
2023
·
IF 7.4
Zhongchun Yuan,Tingting Cao,Min Deng,Jun Ma,Shuo Geng,Chunliang Yang,Yuan Ren,Mengqin Yao,Fei Liu,Xiaodan Wang
It is very crucial but still a huge challenge to develop efficient and durable catalysts to promote hydrogen production from formic acid (FA). Herein, three CeO 2 with structurally well-defined different shapes, i.e., sCeO 2 (spheres), rCeO 2 (rod) and oCeO 2 (octahedral), are prepared, and their effect on the crystal faces and oxygen vacancy over the constructed heterostructure catalysts (Pd-CeO 2 /C) have been intensively investigated in the FA dehydrogenation. Pd-sCeO 2 /C outperforms the other catalysts with a turnover frequency (TOF) value of 2691 h −1 and selectivity to hydrogen of 100 % at 30 °C. A synergism between the CeO 2 (1 1 0) facet and more oxygen vacancies is considered to be key to obtaining the high reactivity. Moreover, biomass carbon promotes the dispersion of Pd-CeO 2 heterostructures due to its large specific surface area and causes more defects in the Pd-CeO 2 /C. Combined with in-situ FTIR and density functional theory (DFT), it is speculated that FA is decomposed through formate pathway over the Pd-sCeO 2 /C. This work thus provides a reasonable design and controllable synthesis strategy for the effective application of FA as an available liquid phase hydrogen storage material.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Huixian Zhou,Yiqing Zeng,Zexian Low,Feng Zhang,Zhaoxiang Zhong,Weihong Xing
Developing cost-effective and high-efficient air purification materials for enhancing the indoor air quality has been an ongoing concern. Herein, MnO 2 /Co–C catalyst layers were wrapped on SiO 2 nanofiber by a combination of thermal pyrolysis and redox reaction method to prepare catalytic membranes (MCCS-x) for the efficient purification of indoor PM and HCHO. The core-dual-shell structure maintains the pore structure of the membrane, providing high gas permeability of 670 m 3 ·m −2 ·h −1 ·kPa −1 . Owing to the introduction of MnO 2 /Co–C enhanced the capture of PM, the optimized MCCS-2 exhibits high filtration efficiency of PM 0.3 and PM 2.5 (99.60% and 99.99%) with a low pressure drop (<80 Pa). In addition, MCCS-2 achieves 100% HCHO removal efficiency at room temperature due to its large specific surface area, high redox property and abundant Mn 4+ and oxygen species. The appropriate proportion of Mn/Co bimetallic sites synergy inhibits the formation of formate and carbonate intermediate species, thus MCCS-2 possesses excellent long-term catalytic stability than contrast sample (MCCS-3 and MS). This work demonstrates a new approach for the fabrication of high-performance catalytic membrane materials for indoor air purification.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Jingjing Niu,Zhe Xue,Jiuchao Tang,Saravanan Rajendran,Xinyu Zhang,Jiaqian Qin
Developing efficient, economic, and environment-friendly electrocatalysts to meet the industrialized hydrogen evolution reaction (HER) needs is highly desired for dealing with the energy crisis. Under the known premise, how to reasonably control the doping amount of copper greatly influences the structure and is one of the key factors affecting the performance of the catalyst. Herein, a series of Ni–Cu–C electrocatalysts are successfully synthesized through a simple electrodeposition method. The unique dendritic morphology can be obtained by adjusting the different glucose concentrations . DFT simulation reveals that the proper proportion of copper can significantly modulate the H adsorption-free energy Δ G H ∗ It can boost the intrinsic activity of Ni–Cu–C catalysts. NCC-3 delivers an overpotential of 87 mV and 165 mV in alkaline media at the current density of 10 mA cm −2 and 100 mA cm −2 , respectively and presents outstanding long-term stability for 50 h. Such excellent HER activity stems from a large ECSA area and better electron-transfer ability. The study presents a feasible way to control metal alloy catalysts' composition in the electrodeposition process .
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JOURNAL OF ELECTRONIC MATERIALS
·
2022
·Vol. 52
·期 2
·1375-1384
·
IF 2.047
Shi Chonghua,Fu Hang,Nie Jiajin,Yao Shaowei
A composite material of Co/N-doped porous carbon was derived from a zeolite imidazolate framework (Zn/Co-ZIF) precursor, which exhibited a controllable microstructure and high specific surface area. In order to study the microwave absorption properties of the composites, the Zn/Co-ZIFs were heat-treated at 930°C in a N 2 atmosphere to obtain the composites, in which Co nanoparticles were distributed uniformly in N-doped porous carbon (Co/C composites). Through N 2 adsorption and desorption testing, the specific surface area of the Co/C composites was about 333.5 m 2 g −1 , and the Barrett−Joyner−Halenda (BJH) pore size distribution was 5.7131 nm, with the majority of pores at mesoporous scale. The microwave absorption properties of Co/C composites with different content were then analyzed, revealing that the Co/C composite with absorbent content of 15 wt.% had the smallest reflection loss (−46.36 dB) at a thickness of 3.1 mm. Based on these results, the Co/C composites not only have the advantages of high specific surface area and special porous structure, but with the appropriate absorbent content, the Co/C composites show excellent microwave absorption performance.
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Catalysts
·
2022
·Vol. 12
·期 12
·1525
·
IF 4.501
Sai Che,Na Ta,Fan Yang,Yulong Yang,Yongfeng Li
Rational design and construction of cost–effective electrocatalysts for efficient hydrogen production has attracted extensive research attention worldwide. Herein, we report the construction of a transition metal selenide/carbon composite catalyst featuring uniform NiSe nanoparticles anchored to single Ni atom doped porous carbon structure (NiSe/Ni–N–C) via a facile one–pot pyrolysis of low–cost solid mixtures. NiSe/Ni–N–C exhibits remarkable catalytic performance towards hydrogen evolution reaction (HER) in 1.0 M KOH, requiring a low overpotential of 146 mV to reach a current density of 10 mA cm−2. The unique carbon layer encapsulation derived from the enwrapping of fluid catalytic cracking slurry further renders NiSe/Ni–N–C excellent for long–term durability in electrolyte corrosion and nanostructure aggregation. This work paves the way for the design and synthesis of highly efficient composite HER electrocatalysts.Keywords:NiSe nanoparticle;single atom catalyst;interfacial electronic engineering;hydrogen evolution reaction
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