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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Nitrogen, sulfur co-doped hierarchical carbon encapsulated in graphene with “sphere-in-layer” interconnection for high-performance supercapacitor

Lihua Cao,Huiling Li,Xiaolin Liu,Shuwu Liu,Lin Zhang,Wenhui Xu,Haoqi Yang,Haoqing Hou,Shuijian He,Yan Zhao,Shaohua Jiang

Rational design of electrode with hierarchical charge-transfer structure and good electronic conductivity is important to achieve high specific capacitance and energy density for supercapacitor, but it still remains a challenge. Herein, a nitrogen, sulfur co-doped pollen-derived carbon/graphene (PCG) composite with interconnected “sphere-in-layer” structure was fabricated, in which hierarchically pollen-derived carbon microspheres can serve as “porous spacers” to prevent the agglomeration of graphene nanosheets. The optimized PCG composite prepared with 0.5 wt% of graphene oxide (PCG-0.5) exhibited high specific capacitance (420   F   g −1 at 1   A   g −1 ), rate performance (280   F   g −1 at 20   A   g −1 ), and excellent cycling stability with 94% of capacitance retention after 10,000 cycles. The symmetrical device delivered a remarkable energy density of 31.3   Wh   kg −1 in neutral medium. Moreover, density functional theory calculation revealed that PCG electrode possessed the accelerated charge transfer and enhanced electronic conductivity, thus ensuring a remarkable electrochemical performance. This work may afford an effective strategy for the development of biomass-derived carbon electrodes with novel charge-transfer structure toward supercapacitor applications.

研究领域: 材料科学 · 能源存储
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Journal of Materials Chemistry A · 2017 ·Vol. 5 ·期 13 ·6245-6256 · IF 8.867

Controllable synthesis of highly uniform flower-like hierarchical carbon nanospheres and their application in high performance lithium–sulfur batteries

Daying Guo,Xi'an Chen,Huifang Wei,Menglan Liu,Feng Ding,Zhi Yang,Keqin Yang,Shun Wang,Xiangju Xu,Shaoming Huang

Elemental sulfur cathodes for lithium/sulfur batteries are receiving intense interest owing to their high theoretical capacity and energy density. However, they still suffer from severe capacity fading and moderate rate capability. Herein, we provide rational design and controllable fabrication of highly uniform flower-like hierarchical carbon nanospheres (FCNS) for sulfur accommodation for lithium/sulfur battery cathodes. The as-prepared three dimension FCNS with a size of around 200 nm seem to be assembled by petal-like carbon nanosheets with a thickness of about 4 nm, forming many mesoporous channels, which lead to their high surface area and large pore volume. With such a tailor-made structure, FCNS/sulfur composite cathodes with high sulfur-loading (81 wt%) deliver high specific capacity, long cycling life and excellent rate capability. Particularly, N-doped flower-like carbon nanospheres (NFCNS) with higher surface area (1223 m2 g−1) and larger pore volume (2.33 cm3 g−1) are also fabricated by treating with NH3 and used to host sulfur in lithium–sulfur battery cathodes, exhibiting more excellent rate capability (829 mA h g−1 at 5C) and cycling stability with a decay of 0.03% per cycle over 200 cycles at 1C. Even though the area density is improved to 2.5 mg sulfur per cm2, the battery still has a decay of 0.056% per cycle over 200 cycles.

研究领域: 材料科学 · 能源存储
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CARBON · 2022 · IF 11.307

Bridging hollow carbon nanostructures to hierarchically pomegranate-like microspheres for efficient oil adsorption and catalysis applications

Danping Tian,Miao Li,Xiaoting Hao,Yajuan Hao,Xiaoming Zhang,Hengquan Yang

Hierarchical carbon superstructures that built from primary nanoscale objects and featured with a micro- or macroscopic architecture are highly desired, as credited by the synergistically integrated specialties. Here, we present a simple “microconfined-assembly-locking” approach to achieve pomegranate-like mesoporous carbon microspheres (PMCMs), in which the Pickering droplet-confined colloidal particle assembly and surfactant-directed interfacial locking are coupled. The formed PMCMs possess a unique micro-nano-hierarchical structure that consisting numerous mesoporous hollow carbon nanospheres within a permeable crust. Benefitting from this hierarchical arrangement, such a peculiar architecture not only preserves high surface area, large pore volume and good accessibility of the nano-building blocks, but also upgrades in mechanical strength and easy handling ability. In addition, this strategy allows the interior microstructures to be manipulated through combinatorial varying the assembled colloidal particles and interfacial chemical locking processes. Notably, the PMCMs show superior sorption capacity and cyclability for organics or oils from water in a fixed-bed system, which could also be applied to enhance the catalytic performance in hydrogenation of aromatic compounds after loading with Ru nanoparticles . This synthetic method provides a powerful bridge between nanoscale objects and microscale patterning, and paves a way to access other novel superstructures for expanding their potential applications.

研究领域: 材料科学 · 环境科学 · 化学工程
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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Selectively anchored vanadate host for self-boosting catalytic synthesis of ultra-fine vanadium nitride/nitrogen-doped hierarchical carbon hybrids as superior electrode materials

Hailun Yang,Pengge Ning,Hongbin Cao,Menglei Yuan,Jianpeng Feng,Jiaxin Yue,Zhenchao Liu,Gaojie Xu,Yuping Li

Hierarchically nanostructured carbon hybrids with highly exposed active sites and specific surface area have been widely researched in high-performed electrochemical capacitors. Inspired from the synergistic effect of uniformly distributed active components and stable carbon substrate, combining with green solvent extraction process, we explored a facile strategy to prepare vanadium nitride quantum dots/nitrogen-doped hierarchical carbon nanocomposites (VNQD/NDHCs) from vanadium aqueous solution, which can provide large pseudocapacitance and excellent electrochemical stability. Vanadate is selective recovered from aqueous solution in form of vanadium-organic compounds (VAORCs) as precursor. Primary amines favor not only the selective metal-polymer coordination, but also the formation of cross-linked carbon matrix. Then, during chemical molecules vapor deposition (CMVD), the vanadate is in-situ nitrided along with the formation of hierarchical carbon. The prepared VNQD/NDHCs-800 exhibits exceptional capacitance (318.3 F g −1 at 1 A g −1 ) and retains 89.7% of the initial capacities after 12000 cycles. SEM and TEM images confirm that a large amount of quantum dots are well embedded in a graphitic carbon matrix, which provides abundant electroactive sites and fast ion diffusion for capacitive storage. This work indicates that it is feasible to directly recovery valuable metals from aqueous solutions to prepare high-performance electrode materials .

CAS / MDL: 124-22-1
研究领域: 材料科学 · 电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Synergistic effect of single-atom Ag and hierarchical tremella-like g-C3N4: Electronic structure regulation and multi-channel carriers transport for boosting photocatalytic performance

Linlin Sun,Yibing Feng,Kai Ma,Xiaohan Jiang,Zhengyang Gao,Jigang Wang,Nan Jiang,Xiaoshuo Liu

It is significant to realize the synergistic effect of single-atom sites and its support to obtain excellent performance photocatalysts. Here, single-atom silver (SAAg) is embedded into the hierarchical tremella-like carbon nitride (3DT-CN) by an efficient one-step reduction method. The photo-degradation mechanism of SAAg/3DT-CN for tetracycline (TC) is first proposed. And the synergistic effect to improve photocatalytic activity is also discussed in depth. Density functional theory (DFT) calculations and physicochemical characterizations reveal that the synergistic effect of SAAg and 3DT-CN has improved the absorption capacity of visible light, the binding energy with oxygen, charge transfer behavior and other properties. Electron spin resonance (ESR) and capture experiments validate the active species involved in the reaction. The first-order kinetic constant of TC degradation by SAAg/3DT-CN is 8.4 times and 3.8 times that of 3DT-CN and AgNP/3DT-CN in 75 min, respectively. This work provides a meritorious structure-activity strategy for the removal of refractory antibiotics.

研究领域: 环境科学 · 材料科学
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Nitrogen-doped hierarchical carbon spheres derived from MnO2-templated spherical polypyrrole as excellent high rate anode of Li-ion batteries

Chunhai Jiang,Jingxia Wang,Zhonghui Chen,Zhiyang Yu,Zhenyu Lin,Zhimin Zou

Hierarchical nitrogen-doped carbon spheres (NCSs) prepared by annealing the MnO 2 -templated spherical polypyrrole (PPy) at 450 or 600   °C were tested as anode materials of Li-ion batteries. The NCSs annealed at 450   °C exhibited higher nitrogen content, more amorphous carbon structure, and lower surface area as compared to the sample annealed at 600   °C. The specific capacities and rate performances of both NCSs samples were much higher than that of commercial mesocarbon microbeads (MCMBs). The NCSs annealed at 600   °C exhibited higher capacity at low current density (<0.5   A   g −1 ) but more rapid capacity decay at elevated current rates referring to the sample annealed at 450   °C. The NCSs annealed at higher temperature also possessed inferior cycling stability, possibly due to its lower electronic conductivity and higher degree of graphitization. A high specific capacity of 250.8   mAh   g −1 was achieved on the NCSs annealed at 450   °C at 3   A   g −1 , demonstrating their high potentiality as anode of high power Li-ion batteries.

研究领域: 材料科学 · 电化学 · 纳米材料 · 能源存储 · 碳材料
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ChemElectroChem · 2020 ·Vol. 7 ·期 9 ·2136-2144 · IF 4.154

Cotton Cloth-Induced Flexible Hierarchical Carbon Film for Sodium-Ion Batteries

Xixue Zhang,Yanhua Wan,Kaiwei Yang,Keming Song,Liwei Mi,Guoqiang Zheng,Xiangming Feng,Weihua Chen

Graphical Through the layers : Cotton cloth-induced flexible hierarchical carbon film is facilely obtained with distinctive carbon nature, unique porous microstructure and crosslinked-network, as flexible substrate for sodium-ion batteries (SIBs). It exhibits favorable flexibility, fast kinetics, and high structural and electrochemical stability, due to predominant surface-controlled reaction mechanism, effective surface chemistry and favorable compatibility with electrolytes. Flexible substrates play a decisive effect on the functions of flexible energy storage devices. However, systematical investigation and understanding of often-used flexible carbon-based substrates is lack. In this work, a reliable cotton cloth induced flexible hierarchical carbon film is facilely obtained. The synthesized-carbonized cotton cloth (SCC) owns distinctive carbon nature with perfect order level and defects, unique porous microstructure, and crosslinked-network. The SCC exhibits favorable flexibility, fast kinetics, high structural and electrochemical durability with high performance (239.4 mAh g −1 and 155.2 mAh g −1 at 0.01 A g −1 in the ether- and ester-based electrolyte in sodium-ion batteries, respectively), superior to commonly-used commercial carbon cloth and graphene film. In addition, the predominant surface-controlled reaction mechanism, effective solid electrolyte interphase and favorable compatible features with different electrolytes are also intensively studied.

CAS / MDL: 7440-66-6
研究领域: 材料科学 · 能源存储技术
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Journal of Energy Storage · 2024 · IF 8.9

Iron doping enhances ZIF-67 based hierarchical carbon bifunction catalyst for oxygen reduction and evolution reactions

Kanjun Sun,Xiaofei Lei,Xuan Xie,Wenjuan Li,Wenbo Hou,Hui Peng,Guofu Ma

Rational design of inexpensive and durable bifunctional oxygen catalysts is essential to facilitate the commercialization of Zn-air batteries. Hence, we report an electrocatalyst with bifunctional catalytic activity, namely Fe species doped into N, S co-doped carbon encapsulated Co catalysts (e-Fe/Co@NSC). Benefiting from the hierarchical porous structure and multiple adsorption sites, the optimized e-Fe/Co@NSC-20 exhibits excellent oxygen evolution reaction (OER) performance, requiring only overpotential of 282 mV to drive a current density of 10 mA cm −2 . More importantly, the e-Fe/Co@NSC-20 also exhibited excellent oxygen reduction reaction (ORR) performance with a half-wave potential of 0.816 V, successfully revealing that it has excellent bifunctional properties. Moreover, Zn-air battery assembled with e-Fe/Co@NSC-20 catalyst as air electrodes have high open-circuit voltage (1.472 V), power density (136 mW cm −2 ) and specific capacity (639 mAh g −1 Zn ), outperforming Pt/C + RuO 2 -based Zn-air battery. This study provides constructive assistance in the design of electrocatalysts with bifunctional properties for Zn-air battery.

CAS / MDL: 1401-55-4 312619-41-3
研究领域: 材料科学 · 电化学 · 能源存储
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Journal of CO2 Utilization · 2022 · IF 8.321

Rationally designed hierarchical carbon supported CuO nano-sheets for highly efficient electroreduction of CO2 to multi-carbon products

Hehua Tang,Yitian Zhou,Yifan Liu,Yao Qian,Zetian Qiu,Anqi Chen,Bo-Lin Lin

Electrochemical reduction of CO 2 to value-added products is a promising path to mitigate CO 2 emissions and achieve renewable energy conversion and storage. Cu-based electrocatalysts can catalyze electrochemical conversion of CO 2 to multi-carbon products, however, low catalytic activity and selectivity have hindered the practical applications of this technology. Rationally designing the structure of catalysts for an improved catalytic performance is of vital importance. Here, we reported a hierarchical phenol formaldehyde resin carbon supported CuO nano-sheets (CuO/PFRC) catalyst for enhanced CO 2 electroreduction to multi-carbon products. Compared with CuO nano-sheets (CuO) and commercial VXC-72r carbon black supported CuO nano-sheets (CuO/XVC), CuO/PFRC showed an enhanced catalytic activity towards multi-carbon products (mainly ethylene). The electrochemical measurements exhibited an ethylene Faradaic efficiency of 47.2 % at − 0.64 V (vs. RHE) with a high partial current density of 599 mA cm −2 , which outperformed most previously reported studies. We proposed that the 3D hierarchical structure of CuO/PFRC could facilitate electron transfer process, thus promoting the catalytic activity. Further study uncovered that the hierarchical CuO/PFRC had higher CO 2 adsorption capacity than control samples, which may favor to form a higher local CO 2 concentration environment during CO 2 electroreduction reaction and further facilitate catalytic activity promotion.

CAS / MDL: 64-17-5
研究领域: 材料科学 · 电化学 · 可再生能源 · 催化
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Boosting photocatalytic degradation of tetracycline under visible light over hierarchical carbon nitride microrods with carbon vacancies

Quanhao Shen,Lingfei Wei,Rehana Bibi,Ke Wang,Dandan Hao,Jiancheng Zhou,Naixu Li

Graphitic carbon nitride is considered as one of the promising photocatalysts for pollution elimination from wastewater. Manipulating the microstructure of carbon nitride remains a challengeable task, which is essential for improving light absorption , separating photogenerated carrier and creating reactive sites. Herein, a carbon vacancy modified hierarchical carbon nitride microrod (CN1.5) has been prepared templated from a melamine-NH 2 OH·HCl complex. The hierarchical microrods are demonstrated to be comprised of interconnected nanosheets with rich carbon vacancies, which endows it with high specific surface area, enhanced light utilization efficiency, available reactive sites, improved charge carrier separation and numerous mass-transport channels. The resultant photocatalyst CN1.5 exhibits an excellent photodegradation efficiency of 87.9% towards tetracycline under visible light irradiation. The remarkable apparent rate constant of 4.91 × 10 −2 min −1 is 7.3 times higher than that of bulk CN. In addition, the degradation pathways are deduced base on the observation of degradation intermediates generating in the photocatalytic process. Mechanism investigation indicates that the major contribution for photodegradation is attributed to ·O 2 – , 1 O 2 and H 2 O 2 species. This work provides new insights into advancing carbon nitride's microstructure to improve photocatalytic degradation performance for highly efficient antibiotic removal and environment remediation.

研究领域: 环境科学 · 材料科学 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Tailoring the three-phase microenvironment surface to induce carbon nitride oxide generating ·O2– with 100% selectivity for ultrafast photodegradation tetracycline under visible light

Xingyu Zhan,Yunxiong Zeng,Jingcai Xu,Yingchun Xia,Xinqing Wang,Fang Tao,Jie Ouyang,Hongliang Li,Liming Yang,Shenglian Luo,Bo Hong

The reactive oxygen species (ROS) contribute to photodegrading tetracycline (TC), which determines the overall efficiency of photocatalysts. Superoxide radical (·O 2 – ) is one of the excellent ROS for photodegrading TC by carbon nitride. However, achieving hierarchical carbon nitride with efficient, stabile, and selective production of ·O 2 – via O 2 photoreduction is a great challenge. Herein, a carbon nitride oxide nest (CNON 6 ) with carbon/nitrogen vacancies (C-v, N-v) and oxygen substitution (O-s) was prepared via tailoring surface microenvironment. The CNON 6 can photodegrade 82% of TC within 2 min under visible light, and the pseudo-first-order kinetic constant is 1.22 min −1 , 24-fold higher than that of CN. The superior photoactivity is attributed to a unique surface microenvironment, which N-v increased photoelectric conversion efficiency, C-v enhanced O 2 adsorption and O-s induced ·O 2 – evolution with ∼ 100% selectivity. Moreover, PVDF membrane-supported CNON 6 (11.33 cm 2 , 0.88 mg/cm 2 ) can completely remove TC from wastewater at a rate of 2.62 mg/h in a simulated industrial continuous flow cell. The cost-effectiveness assessment was $6.36/kg/h, implying the CNON 6 /PVDF has a bright application prospect in wastewater treatment. This work developed a surface microenvironment tailor strategy to design photocatalysts for efficient degradation of TC.

CAS / MDL: 57-13-6 298-83-9 64-75-5
研究领域: 环境科学 · 材料科学 · 化学工程 · 光催化
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ACS Nano · 2019 · IF 13.903

Highly Dispersed Catalytic Co3S4 among a Hierarchical Carbon Nanostructure for High-Rate and Long-Life Lithium–Sulfur Batteries

Hui Zhang,Mingchu Zou,Wenqi Zhao,Yunsong Wang,Yijun Chen,Yizeng Wu,Linxiu Dai,Anyuan Cao

Lithium–sulfur (Li–S) batteries are next-generation energy storage systems with high energy density, and the rate performance is a very important consideration for practical applications. Recent approaches such as introducing catalytic materials to facilitate polysulfide conversion have been explored, yet the results remain unsatisfactory. Here, we present an optimized Li–S electrode featured by a large amount of highly dispersed Co3S4 nanoparticles (∼10 nm in size) throughout a hierarchical carbon nanostructure hybridized from ZIF-67 and carbon nanotube (CNT) sponge. This enables homogeneous distribution and close contact between infiltrated sulfur and Co3S4 nanoparticles within the ZIF-67-derived N-doped carbon nanocubes, leading to effective chemical interaction with polysulfides, maximum catalytic effect and enhanced lithium ion diffusion, while the built-in three-dimensional CNT network ensures high electrical conductivity of the electrode. As a consequence, the Li–S battery exhibits both extraordinary rate performance by maintaining a capacity of ∼850 mAh g–1 at very high charge/discharge rate (5 C) and long-term cycling stability with 85% retention after 1000 cycles at 5 C (an average capacity fading rate of only 0.0137% per cycle).

CAS / MDL: 75-15-0 10026-22-9
研究领域: 材料科学 · 能源存储 · 电化学 · 纳米技术
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