ACS Applied Energy Materials
·
2023
·
IF 6.4
Zeqing Hu,Rong Wei,Chen Yan,Han Wan,Yu Liu,Longjiu Cheng,Zhou Li,Jiming Song
In this work, carrier concentration optimization and effective mass increase of Cu2GeSe3, which were considered to be a synergetic effect of electrical transport properties, were achieved by the co-doping of Bi and Zn on the Cu site. This effect led to a higher Seebeck coefficient of ∼307.76 μV K–1 at 723 K for the Cu1.988Bi0.01Zn0.002GeSe3 sample. This effect also resulted in a higher power factor of ∼8.66 μW cm–1 K–2 at 723 K and an average power factor of ∼6.29 μW cm–1 K–2 at the temperature range of 303–723 K for the Cu1.988Bi0.01Zn0.002GeSe3 sample, which were ∼135 and ∼196% larger than those of pristine Cu2GeSe3, respectively, and are among the highest value of the Cu2GeSe3-based sample. Benefiting from simultaneous optimization of the power factor, the maximum ZT of ∼0.75 for the Cu1.988Bi0.01Zn0.002GeSe3 sample at 723 K was obtained, which is ∼288% higher than that of Cu2GeSe3.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Dongdong Xu,Zhigao Xue,Lei Han,Kai Tao
Bimetallic sulfides with superior electrochemical activity are extensively explored as electrode materials for electrochemical energy related applications. However, their utilizations are impeded due to unfavorable faradaic reaction kinetics and poor electrochemical stability. To overcome these defects, this study reports interface engineering of heterogeneous nanosheet arrays on Ni foam (NF) through surface modification of metal-organic framework (MOF)-derived zinc cobalt sulfide (Zn/Co-S) with CeO 2 nanoparticles (NPs). MOF-derived porous Zn/Co-S nanosheets have highly exposed electrochemical active sites and abundant channels for charge transport. The strong interfacial coupling between Zn/Co-S and defective CeO 2 leads to fast charge transfer, thereby improving electrochemical activity. The CeO 2 can also prevent Zn/Co-S from degrading in KOH solution. Moreover, the self-supported electrode shows high electronic conductivity and strong adhesion with the conductive substrate. Therefore, the specific capacity and electrochemical stability of resulting Zn/Co-S@CeO 2 /NF are significantly higher compared with Zn/Co-S/NF. Furthermore, an asymmetric supercapacitor (ASC) based on Zn/Co-S@CeO 2 /NF and activated carbon (AC) exhibits high energy storage capability (42.4 Wh kg −1 ) and outstanding operating durability (91.1 % after 8000 cycles). These results demonstrate that the as-prepared electrode is a superior candidate for electrochemical devices .
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Small
·
2023
·Vol. 19
·期 20
·2207569
·
IF 13.3
Yakun Tian,Ming Wen,Aijian Huang,Qingsheng Wu,Zhiguo Wang,Quanjing Zhu,Tao Zhou,Yongqing Fu
High stability and efficiency of electrocatalysts are crucial for hydrogen evolution reaction (HER) toward water splitting in an alkaline media. Herein, a novel nano-Pt/Nb-doped Co(OH) 2 (Pt/Nb Co(OH) 2 ) nanosheet is designed and synthesized using water-bath treatment and solvothermal reduction approaches. With nano-Pt uniformly anchored onto Nb Co(OH) 2 nanosheet, the synthesized Pt/Nb Co(OH) 2 shows outstanding electrocatalytic performances for alkaline HER, achieving a high stability for at least 33 h, a high mass activity of 0.65 mA µg −1 Pt, and a good catalytic activity with a low overpotential of 112 mV at 10 mA cm −2 . Both experimental and theoretical results prove that Nb-doping significantly optimizes the hydrogen adsorption free energy to accelerate the Heyrovsky step for HER, and boosts the adsorption of H 2 O, which further enhances the water activation. This study provides a new design methodology for the Nb-doped electrocatalysts in an alkaline HER field by facile and green way.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hao Zhang,Guanghui Guo,Ziyue Wang,Qian He,Xiaohui He,Hongbing Ji
Cost-effective catalysts for the complete oxidation of formaldehyde (HCHO) are essential for indoor air purification and human health. Here, we report a precursor atomization strategy to synthesize cobalt single-atom catalysts (Co SACs), and the Co SACs show complete conversion of 50 ppm HCHO at room temperature and the catalysts are stable during at least 120 h. The HCHO oxidation activity of Co SACs outperforms all the reported non-noble catalysts at room temperature. DFT calculations and isotope experiments reveal the mechanism of HCHO removal over Co SACs that the decomposition of formate intermediates is the kinetically rate-determining step. The excellent formate intermediate decomposition ability of Co SACs is the key factor in achieving excellent HCHO oxidation performance. Considering the facile and versatile SACs synthesis approach, remarkable performance in HCHO abatement, as well as cheap cost, it is believed that this study may open a window for Co SACs industrial application.
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Chemistry-An Asian Journal
·
2023
·Vol. 18
·期 10
·e202300150
·
IF 4.1
Lianghao Song,Jing Zhang,Chengyu Huang,Chenfei Zhao,Xuemin Yin,Hongli Long,Yang Liu,Yufeng Zhao
Graphical A novel ZIF-assisted strategy was developed to synthesize Co nanoparticles loaded on mesoporous N-doped carbon support of hollow cubic nanobox constructed by pyrolysis of TA-treated ZIF-67 at high temperature. The Co−NC-800 NBs-based ZABs present higher power density and better stability than commercial Pt/C catalysts. Design of non-noble metal electrocatalysts with high catalytic activity and stability to replace commercial Pt/C is crucial in the commercialization development of Zn-air batteries (ZABs). In this work, Co catalyst nanoparticles coupled with nitrogen-doped hollow carbon nanoboxes were well designed through zeolite-imidazole framework (ZIF-67) carbonization. As a result, the 3D hollow nanoboxes reduced the charge transport resistance, and the Co nanoparticles loaded on nitrogen-doped carbon supports exhibited excellent electrocatalytic performance for oxygen reduction reaction (ORR, E 1/2 =0.823 V vs . RHE), similar to that of commercial Pt/C. Moreover, the designed catalysts showed an excellent peak density of 142 mW cm −2 when applied on ZABs. This work provides a promising strategy for the rational design of non-noble electrocatalysts with high performance for ZABs and fuel cells.
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Crystals
·
2023
·Vol. 13
·期 3
·460
·
IF 2.7
Danni Huang,Tong Xiao,Beibei Fu,Shoulei Xu,Yuyang Huang,Wen Deng,Zhukun Zhou
ZrO2is an attractive host matrix for luminescence material because of its excellent physical properties, such as low phonon energy and wide band gap. In this work, the highly transparent Tm2O3and Yb2O3co-doped yttria stabilized zirconia (YSZ) (abbreviated as Yb/Tm: YSZ) single crystals were grown by the optical floating zone method. The Yb/Tm: YSZ samples were stabilized in the cubic phase at room temperature when Yb3+and Tm3+replaced Y3+. The influence of Yb3+co-doping on the up-conversion luminescence properties of the crystals was systematically studied. A total of 0.5 mol% Tm2O3and 2.0 mol% Yb2O3co-activated YSZ single crystal (abbreviated as 2.0Yb/Tm: YSZ) has the maximum luminous intensity. There were seven absorption peaks located at around 358, 460, 679, 783.3, 850–1000, 1200, and 1721.5 nm that were observed in the absorption spectrum of the 2.0Yb/Tm: YSZ single crystal. There were three up-conversion peaks at around 488, 658 and 800 nm that were observed when the Yb/Tm: YSZ samples were excitated at 980 nm. The fluorescence lifetime of Tm3+for the1G4→3H6transition of the 2.0Yb/Tm: YSZ sample is 7.716 ms as excited with a 980 nm laser. In addition, the oscillator strength parameters Ωλ(λ = 2, 4 and 6) of this sample were derived by the Judd–Ofelt theory to evaluate the laser performance of the host materials. The ratio Ω4/Ω6of this sample is 0.80, implying its excellent laser output. Therefore, the 2.0Yb/Tm: YSZ single crystal is a considerable potential material for laser and luminescence applications.Keywords:YSZ single crystal;Yb3+and Tm3+co-activated;optical floating zone method;up-conversion luminescence;Judd–Ofelt theory
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TRANSITION METAL CHEMISTRY
·
2023
·Vol. 48
·期 2
·125-133
·
IF 1.7
Hu Yi,Xu Jingsong,Zhang Tianzhu,Zhong Hang,Chen Jun,Liu Xinai,Pan Qifa,Liu Ruidong,Jiang Chunli,Chen Jun
Electrocatalytic water splitting to produce hydrogen is a promising route to provide green hydrogen on a large scale. To explore non-noble metal electrocatalysts with high performance is still a challenge. Herein, a one-step electrodeposition way is developed to construct the heterostructural (NiO-La 2 O 3 )/(Ni-La)/NiO/Ni electrocatalysts on Ni foam. The dark Ni-La coating was prepared by co-electrodeposition from an aqueous solution containing LaCl 3 and NiCl 2 with a molar concentration ratio of 1:5. Among these heterostructural Ni-based electrocatalysts, an excellent HER activity is achieved: an overpotential of 22 mV at the current density of 10 mA cm −2 in 1 M KOH solution. It is demonstrated that the introduction of La significantly reduces the overpotential for HER. The higher the La content in the Ni-La coating of these electrocatalysts, the better the electrocatalytic HER performance was exhibited. This work provides a facile and inexpensive route to prepare Ni-La coating on electrodes in an aqueous solution.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Liuxin Xu,Ya Pan,Hongmei Li,Ruichao Xu,Zhihu Sun
The presence of interfacial sites between Pt-group metals and transition metal oxides can effectively improve the catalytic activity of Pt-group catalysts, but under moisture-rich conditions they suffer from severe deactivation due to water poisoning of the active sites. Here, we propose for the first time a Lanthanum (La)-doping strategy to improve the water-resistance of the Pt-based catalysts. We synthesized a Pt-CoO/Al 2 O 3 catalyst that is active for CO oxidation under dry conditions but deactivates rapidly under moisture. This rapid deactivation is overcome by La-doping, which delivers boosted activity (100 % CO conversion at 15 °C) and long-term on-stream stability. In situ X-ray absorption fine-structure and in situ diffuse reflectance infrared Fourier transform spectra revealed that the doped La, in the form of La 2 O 3 , plays dual roles of suppressing the carbonate formation on the active sites and modifying the electronic structure of Pt. The synergetic effects between La 2 O 3 and the active Pt−O−Co interfacial sites in La-doped Pt-CoO/Al 2 O 3 lead to the outstanding activity under the moisture-rich condition.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Huaqi Wang,Chenghong Sun,Enze Zhu,Chaoyang Shi,Jie Yu,Mingli Xu
Metal–organic framework (MOF)-derived carbon materials have emerged as important candidates in the field of catalysis because of their simple synthesis, easy construction, good conductivity, and high catalytic activity. Fe 3 C nanoparticles prepared from MOFs facilitate the catalytic activity of adjacent single atoms and exhibit powerful catalytic properties. In this work, a composite structured catalyst with Fe 3 C, Co nanoparticles, and M-N x single atoms (M = Co, Fe) was synthesized (denoted as Fe 3 C-Co-NC) by constructing Fe-doped bilayer zeolitic imidazolate frameworks (ZIFs) with a core–shell structure, which were used as bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). The Fe 3 C-Co-NC catalyst exhibits superior half-wave potential ( E 1/2 = 0.89 V) and overpotential ( E j=10 = 1.67 V) and outperforms the commercial Pt/C and RuO 2 . This result can be attributed to the high specific surface area, hierarchical pore structure , and high graphitization degree of the Fe 3 C-Co-NC catalyst, especially the synergistic effect between Fe 3 C and adjacent single-atom active sites. Specifically, the Zn–air battery assembled using the Fe 3 C-Co-NC catalyst displays high peak power density (203 mW cm −2 ) and specific capacity (815 mAh g −1 ) without degradation after charge/discharge cycles for 57 h. Therefore, this work offers important insights into the design and research of high-performance ORR/OER bifunctional catalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Fangfang Liu,Jinan Niu,Xiuyun Chuan,Yupeng Zhao
At present, the designs of carbon nanomaterials are indispensable to fulfill the growing demand for high energy and power density of energy storage devices. Heteroatom-doped (such as B, N, O, P, S, etc) porous carbon has great potential in the application of supercapacitor (SC) electrode materials. Nitrogen-doped carbon (N-C) has displayed superior properties in SC applications, which has attracted the attention of researchers. Due to the synergistic effect between N and S atoms, the nitrogen and sulfur co-doped carbon (N/S-C) shows superior electrochemical properties compared to the nitrogen single-doped porous carbon. Therefore, the development of N/S-C as SC electrode is of great importance. In recent years, the literature on the study of N-C for SC applications has been very extensive, however, there are a limited number of review articles on N/S-C. This manuscript represents future research directions, recent developments in the preparation of N/S-C and its application in SC. Herein, the preparation and dimension structure of N/S-C were summarized. Finally, the electrochemical properties including specific capacitance (C F ), energy density (ED) and power density (PD) are critically reviewed when these N/S-C are used as SC electrodes.
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JOURNAL OF POLYMER SCIENCE
·
2023
·Vol. 61
·期 17
·2025-2036
·
IF 3.4
Tao Li,Zhijian Liu,Yao Chen,Na Sun,Haozhou Shu,Lili Wu,Chaocan Zhang,Dong Xie
Two-component catalysts composed of tetra ( para -X substituted) phenylporphyrin aluminum (III) chloride, T ( p -X-P)PAlCl, (where X = H, F, Cl, Br, CH 3 , OCH 3 , tert -butyl), and cocatalyst bis(triphenylphosphine)imminium chloride (PPN + Cl − ), could initiate the polymerization of propylene oxide (PO). And they could react with rac -lactide, ( rac -LA), in the presence of propylene oxide (PO), to yield chains of enriched isotactic polylactide (PLA) with trace polyether segment. Also, these catalysts displayed different catalytic activity in the copolymerization of CO 2 and PO, resulting in poly(carbonate-co-ether) copolymer with different carbonate unit content (CU%). Further, these catalysts could initiate one-pot regio- and stereo- selective terpolymerization of rac -LA, CO 2 and rac -PO, resulting in multi-blocky poly(carbonate-co-lactide) with trace polyether segment. The structure of the products was verified by 1 H NMR, 13 C NMR, GPC, and DSC analysis, and it was found that variation of substitution groups in the periphery of porphyrin ligand would affect on the catalytic efficiency of ter-polymerization, and the relative polymerization reaction ratio of the ring-opening polymerization of LA (ROP) to the ring-opening copolymerization of PO and CO 2 (ROCOP), resulting in ter-polymer with different contents of PLA segment and PPC segment. However, H-T % in polycarbonate unit and P i % in polylactide unit did not vary much with the change of catalysts. Graphical
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Small
·
2023
·Vol. 19
·期 35
·2300663
·
IF 13.3
Qing Hou,Ajuan Hu,Hongbin Ni,Zongqiang Sun,Jianing Duan,Xiaoming Xu,Jingmin Fan,Ruming Yuan,Mingsen Zheng,Quanfeng Dong
As a holy grail in electrochemistry, both high-power and high-energy electrochemical energy storage system (EES) has always been a pursued dream. To simultaneously achieve the “both-high” EES, a rational design of structure and composition for storage materials with characteristics of battery-type and capacitor-type storage is crucial. Herein, fluorine-nitrogen co-implanted carbon tubes (FNCT) have been designed, in which plentiful active sites and expanded interlayer space have been created benefiting from the heteroatom engineering and the fluorine-nitrogen synergistic effect, thus the above two-type storage mechanism can get an optimal balance in the FNCT. The implanted fluorine heteroatoms can not only amplify interlayer spacing, but also induce the transformation of nitrogen configuration from pyrrole nitrogen to pyridine nitrogen, further promoting the activity of the carbon matrix. The extraordinary electrochemical performance as results can be witnessed for FNCT, which exhibit fast lithium-ion storage capability with a high energy density of 119.4 Wh kg −1 at an ultrahigh power density of 107.5 kW kg −1 .
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