JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Peng Song,Congcong Li,Ningmiao Zhao,Zhenyuan Ji,Linzhi Zhai,Xiaoping Shen,Qi Liu
Carbon nanosheets with heteroatom doping and well-developed porosity exhibit broad application foreground for Zn-ion hybrid supercapacitors (ZHSCs), but the simple and controllable preparation is still of great challenge. In this study, by using LiCl-KCl as in-built templates, histidine as carbon and nitrogen sources, and KNO 3 , K 2 SO 4 , KOH or Na 2 S 2 O 3 as active agent, a series of N and N S doped porous carbon nanosheets are developed. Results indicate that, with the activator introduction, pore structures of the carbonized products are notably boosted, showing an astounding 30–244 % increase in BET specific surface area, and meanwhile, heteroatom with a content of ca. 12 % can be doped into the resultant carbon skeletons. Specifically, the NSPCN-800 (activated by Na 2 S 2 O 3 ) with a large specific surface area of 1297 m 2 /g, a hierarchically porous structure composed of abundant micropores and mesopores, and a suitable heteroatom content (N: 11.9 wt%; S: 0.6 wt%) presents an impressive energy storage behavior as cathode for ZHSCs, including a specific capacitance of 165.8F/g, a specific capacity of 95.2 mAh/g, an energy density of 59.0 Wh kg −1 and a cyclic stability with a 82.6 % capacity retention after 5000 cycles. These performance parameters surpass numerous reported ZHSCs, making NSPCN-800 a very promising cathode for practical use.
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高影响因子
iScience
·
2023
·
IF 5.8
Song Wei,Caichao Wan,Xingong Li,Jiahui Su,Wenjie Cheng,Huayun Chai,Yiqiang Wu
Summary Traditional electrode materials still face vital challenges of few active sites, low porosity, complex synthesis process, and low specific capacitance. Herein, N-doped and 3D hierarchical porous graphene nanofoam (N-GNF) is created on carbon fibers (CFs) by employing a facile, fast, and environmentally friendly strategy of N 2 plasma activation. After an appropriated N 2 plasma activation, the graphene nanosheets (GNSs) synthesized by Ar/CH 4 plasma deposition transform into N-GNF successfully. N doping donates rich active sites and increases the hydrophilia, while hierarchical nanoarchitecture exposes an enlarged effective contact area at the interface between electrode and electrolyte and affords sufficient space for accommodating more electrolytes. The as-assembled flexible N-GNF@CFs//Zn NSs@CFs Zn ion capacitor delivered a high energy density of 105.2 Wh kg −1 at 378.6 W kg −1 and initial capacity retention of 87.9% at the current of 2 A g −1 after a long cycle of 10,000.
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高影响因子
Nanoscale
·
2022
·Vol. 15
·期 3
·1172-1179
·
IF 8.307
Yuemei Liu,Junhong Ma,Tuan K. A. Hoang,Lijing Yang,Zhaohui Chen
NiFe-based nanoparticles attached to heteroatom-doped carbon are found to act as tremendously efficient oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) electrocatalysts. Nevertheless, it is extremely challenging to control the particle size and avoid aggregation. Herein, nitrogen-doped carbon encapsulated Ni3Fe nanoparticles (Ni3Fe@NC) are prepared by two-stage pyrolysis with a low rate based on the in situ structural evolution of FeNi-PBAs. The strategy results in uniform Ni3Fe nanoparticles anchoring within the carbon shell and thus facilitating interfacial interaction. Benefiting from the enhanced synergism between Ni3Fe particles and NC layers, Ni3Fe@NC-600 demonstrates the best catalytic activity and durability, not only with almost the same onset potential (1.01 V) as commercial Pt/C for the ORR but also satisfactory OER performance with a low overpotential of 0.29 V at 10 mA cm−2 in 0.1 M KOH. Moreover, the Zn–air battery assembled using the Ni3Fe@NC-600 cathode exhibits superior performance to commercial Pt/C + RuO2. The simple and scalable method of this work provides insight into the fabrication of high-performance and cost-effective bifunctional oxygen electrocatalysts.
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Small
·
2022
·Vol. 19
·期 8
·2206478
·
IF 15.153
Yuting He,Yufei Jia,Baozhu Yu,Yi Wang,Hongtao Li,Yongning Liu,Qiang Tan
Platinum group metal (PGM)-free M-N-C catalysts have exhibited dramatic electrocatalytic performance and are considered the most promising candidate of the Pt catalysts in oxygen reduction reaction (ORR). However, the electrocatalytic performance of the M-N-C catalysts is still limited by their inferior intrinsic activity and finite active site density. Regulating the coordination environment and increasing the pore structure of the catalyst is an effective strategy to enhance the electrocatalytic performance of the M-N-C catalysts. In this work, the coordination environment and pore structure exquisitely regulated Fe-N-C catalyst exhibit excellent ORR activity and durability. With the enhanced intrinsic activity and increased active site density, the optimized Fe-N/S-C catalyst shows impressive ORR activity ( E 1/2 = 0.904 V vs reversible hydrogen electrode (RHE)) and superior long-term durability in an alkaline medium. As the advanced physical characterization and theoretical chemistry methods illustrate, the S-modified Fe-N x (Fe-N 3 /S-C) moiety is confirmed as the improved active center for ORR, and the increased active site density further improved ORR efficiency. Based on the Fe-N/S-C cathode, a Zn-air battery is fabricated and shows superior power density (315.4 mW cm −2 ) and long-term discharge stability at 20 mA cm −2 . This work would open a new perspective to design atomically dispersed iron-metal site catalysts for advanced electro-catalysis.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Jingshun Shen,Qi Liu,Qiqi Sun,Jianwei Ren,Xue Liu,Zuoxu Xiao,Chuanwang Xing,Yuexing Zhang,Guangwu Yang,Yanli Chen
A novel two-dimensional (2D) single-atom Fe/N/C catalyst (Fe 1 Zn 30 NC PDI ) has been prepared upon pyrolyzing a well-designed quasi-Fe-/Zn-phthalocyanine-based polymer (qFePc 1 @qZnPc 30 @PDI). In the qFePc 1 @qZnPc 30 @PDI precursor, qFePc moieties containing Fe-N 4 sites are efficiently segregated by lots of qZnPc moieties connected together by perylene linkers, which not only leads to the larger specific area in the resulting Fe 1 Zn 30 NC PDI but more importantly ensures the in-situ formation of Fe-N 4 sites on the self-supporting 2D N-doped carbon backbone. Impressively, Fe 1 Zn 30 NC PDI exhibites its superior oxygen reduction reaction (ORR) electro-catalytic activity and peroxidase (POD)-like activity. For ORR in an alkaline medium, it exhibites a much higher onset potential of 0.97 V and half-wave potential of 0.89 V than 20 wt% Pt/C catalyst with good durability of 92 % retention rate after 20000 s. And, Fe 1 Zn 30 NC PDI also shows better peak power density (86 mW cm −2 ) compared with 20 wt% Pt/C in Zn-air battery. Benefiting from the specific POD-like activity of Fe-N 4 , the Fe 1 Zn 30 NC PDI also shows excellent and selective performance in colorimetric H 2 O 2 sensing, with the ultrafast response (30 s), a low limit of detection (10 nM), and good robustness. This work sheds light on a promising design concept for synthesizing 2D polymer-derived single-atom multifunctional catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Chongshang Guan,Tian Hou,Wuyang Nie,Qian Zhang,Libing Duan,Xiaoru Zhao
In this work, different BiOBr powders (without and with Zn doping) were prepared. Their specific properties and photocatalytic performance were studied. Zn doped BiOBr showed higher carrier transportation ability, beneficial to high performance photocatalysis . Further analysis and theoretical calculations unveiled that Zn doping resulted in more dispersive energy band structure with improved oxygen vacancy (O V ) generation due to lattice distortion. O V acted as trap centers, playing dominant role in carrier transportation enhancement, which also synergized with more dispersive energy band due to Zn doping, improving carrier separation and transfer. Besides, Zn doping would further strengthen trapping effect under O V existence, stimulating synergistic enhancement to spatial charge separation and transfer with O V . With synergy of Zn doping and O V , Zn doped samples produced 1.75 times higher CH 4 generation during gas–solid photocatalytic reduction of CO 2 under visible light , testifying successful conducting of Zn doping improved photocatalytic capacity on BiOBr.
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ACS Catalysis
·
2022
·
IF 13.7
Yuting He,Xiaoxuan Yang,Yunsong Li,Liting Liu,Shengwu Guo,Chengyong Shu,Feng Liu,Yongning Liu,Qiang Tan,Gang Wu
Single-metal site catalysts have exhibited highly efficient electrocatalytic properties due to their unique coordination environments and adjustable local structures for reactant adsorption and electron transfer. They have been widely studied for many electrochemical reactions, including oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). However, it remains a significant challenge to realize high-efficiency bifunctional catalysis (ORR/OER) with single-metal-type active sites. Herein, we report atomically dispersed Fe–Co dual metal sites (FeCo–NC) derived from Fe and Co co-doped zeolitic imidazolate frameworks (ZIF-8s), aiming to build up multiple active sites for bifunctional ORR/OER catalysts. The atomically dispersed FeCo–NC catalyst shows excellent bifunctional catalytic activity in alkaline media for the ORR (E1/2 = 0.877 V) and the OER (Ej=10 = 1.579 V). Moreover, its outstanding stability during the ORR and the OER is comparable to noble-metal catalysts (Pt/C and RuO2). The atomic dispersion state, coordination structure, and the charge density difference of the dual metal site FeCo–NC were characterized and determined using advanced physical characterization and density functional theory (DFT) calculations. The FeCo–N6 moieties are likely the main active sites simultaneously for the ORR and the OER with improved performance relative to the traditional single Fe and Co site catalysts. We further incorporated the FeCo–NC catalyst into an air electrode for fabricating rechargeable and flexible Zn–air batteries, generating a superior power density (372 mW cm–2) and long-cycle (over 190 h) stability. This work would provide a method to design and synthesize atomically dispersed multi-metal site catalysts for advanced electrocatalysis.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 26
·40041-40052
·
IF 5.19
Luo Qin,Huang Xiaofeng,Deng Qiulin,Zhao Xueyuan,Liao Huiwei,Deng Hongquan,Dong Faqin,Zhang Tao,Shi Lianjun,Jiang Jinlong
The photocatalytic properties of Zn/Co zeolite imidazolate frameworks (ZIF-ZnCo) prepared by various Zn/Co ratio are of significantly diversity due to the morphology structure of the ZIF-ZnCo. Thereinto, the prepared ZIF-ZnCO-8:1 is excellent capability by virtue of its 3D cross-shaped structure. Spectral test results show that as-prepared novel 3D cross-shaped ZIF-ZnCo has a lower recombination rate of electron and hole pairs than the lamellar and dodecahedral, thus improving the photocatalytic ability. The photocatalytic ability of 3D cross-shaped ZIF-ZnCo was carefully investigated for removing mixed solution of Congo Red (CR) and Cr(VI). The photocatalytic reduction ability of 3D cross-shaped ZIF-ZnCo was 22% higher than ZIF-8 for Cr(VI). Meanwhile, CR was altogether removed at dark processing and Cr(VI) was removed 70% after dark processing 120 min and photocatalytic 240 min. Therefore, the high adsorption and photocatalytic capacity denote the potential application of 3D cross-shaped ZIF-ZnCo. Graphical abstract
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Deyu Wang,Yongfu Kang,Lei Lei,Yoann de Rancourt de Mimérand,Xiaoyun Jin,Jia Guo
In this study, we explore the potential of an innovative method based on cold plasma discharge (CPD), to fabricate stable supported photocatalysts for the photodegradation of organic water pollutants. Supported catalysts bear significant advantages compared to colloidal ones, the main benefit being that they can be separated from water and reused much more easily, which is a crucial aspect especially of nanocompounds. They can also participate in reducing catalyst loss between operations or even enable continuous-flow processes, usually more productive than batch, discontinued operations. Hereby, we describe an immobilization approach, i.e. in situ complexation-assisted precipitation (ISCAP), which allows the fabrication of nanoCdS photocatalyst, directly at the surface of a polymer substrate. More specifically, we establish the potential of this process to obtain a hybrid coating of zinc-doped CdS, in situ . Our findings revealed that the resulting supported catalyst was photoactive – degrading Rhodamine B (RhB) dye, easily recyclable and photostable thanks to the successful doping of the catalytic phase. In addition, it seems that the immobilization itself stabilized the catalyst, probably thanks to polyvinylphosphonic acid (PVPA), used as a complexing and binding agent. The catalytic phase was immobilized on a resin substrate that was fabricated by liquid crystal diode (LCD) 3D printing, and conceived using fractal-inspired geometry.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Tuo Xin,Yiran Wang,Qiuju Xu,Jiaxiang Shang,Xiangcheng Yuan,Weixing Song,Jinzhang Liu
Rechargeable aqueous zinc-ion batteries (ZIBs) hold great promise for future applications in large-scale energy storage systems. However, the rampant dendrite growth and undesired hydrogen gas evolution over the Zn anode are key issues that make the current ZIB technology immature. Herein, we demonstrate the use of a zeolitic imidazolate framework (ZIF)-derived composite coating on Zn foil for simultaneously suppressing the dendrite growth and H2 evolution when operated in ZnSO4 electrolytes. The polyhedral ZIF-8 granules are converted into mesoporous N-doped carbon (NC) decorated with ZnS nanoparticles, and this ZnS/NC composite is coated onto Zn foil. For comparison, bare Zn anodes and Zn foils coated with other ZIF-derived materials including ZnS nanocrystals and NC frameworks are also used to make half or full cells. The Zn@ZnS/NC anode shows the best performance in terms of superb cycling stability, suppressed dendrite growth, and reduced H2 evolution. At the interface between ZnS/NC coating and Zn foil, confined parasitic reactions result in a layer of an amorphous ZnO nanosheet network, which has a positive effect on reducing water activity. The role of this amorphous ZnO byproduct in reducing H2 evolution is discussed in detail. This work sheds light on a strategy for making practical ZIBs.
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Energy Technology
·
2022
·Vol. 10
·期 5
·2200057
·
IF 4.149
Yuebing Wang,Ruowei Yi,Aling Chen,Can Fang,Yaping Wang,Qingfeng Yi,Meiyang Liu,Shijie Liu,Shaoqi Zhan,Bin Zhong
Herein, we synthesize Fe-based nanocatalysts supported on the composites composed of hollow carbon spheres (HCSs) and metal–organic frameworks (MOFs) by a facile pyrolysis method. The composites with different ratios of HCSs and MOFs present an interesting phenomenon: the oxygen reduction reaction (ORR) limiting current increases along with the HCSs content, while the onset potential and half-wave potential show the highest values when the ratio between HCSs and MOFs is optimized. The composite catalysts exhibit superior ORR electrocatalytic performance than Pt/C in alkaline and neutral media. Even in the acidic media, these composite catalysts still present a close catalytic activity to Pt/C. For the oxygen evolution reaction (OER) test, the prepared Fe-NC@NHCS-600 shows a reduced overpotential to that of the benchmark IrO 2 . The rechargeable Zn-air battery using Fe-NC@NHCS-600 as the catalyst of air electrode exhibits superior discharge capability with an open-circuit voltage of 1.620 V and a maximum power density of 278.97 mW cm −2 in alkaline electrolyte, as well as an open-circuit voltage of 1.457 V and a maximum power density of 114.96 mW cm −2 in neutral electrolyte. The battery also exhibits steady cycling stability for more than 90 and 70 h at 5 and 10 mA cm −2 , respectively.
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Small
·
2022
·Vol. 18
·期 44
·2204827
·
IF 15.153
Qing Cao,Zhaoyang Cheng,Jiajun Dai,Tianxiao Sun,Guixiang Li,Lili Zhao,Jiayuan Yu,Weijia Zhou,Jianjian Lin
The rational design for transition metals-based carbon nano-materials as efficient electrocatalysts still remains a crucial challenge for economical electrochemical hydrogen production. Carbon nanotubes (CNTs) as attractive electrocatalysts are typically activated by non-metal dopant to promote catalytic performance. Metals doping or metal/non-metal co-doping of CNTs, however, are rarely explored. Herein, this work rationally designs bimetal oxide templates of ZnCo 2 O 4 for heterogeneously doping Zn and N into Co nanoparticles embedded carbon nanotubes (Co@Zn-N-CNTs). During the formation of CNTs, Zn atoms volatilize from ZnCo 2 O 4 and in situ dope into the carbon skeleton. In particular, owing to the low electronegativity of Zn, the electrons aptly transfer from Zn to carbon atoms, which generate a high electron density for the carbon layers and offer more preponderant catalytic sites for hydrogen reduction. The Co@Zn-N-CNTs catalyst exhibits enhanced hydrogen evolution reaction activity in 0.5 m H 2 SO 4 electrolyte, with a low onset potential of −20 mV versus RHE at 1 mA cm −2 , an overpotential of 67 mV at 10 mA cm −2 , a small Tafel slope of 52.1 mV dec −1 , and persistent long-term stability. This study provides brand-new insights into the utilization of Zn as electronic regulator and activity promoter toward the design of high-efficiency electrocatalysts.
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