ChemSusChem
·
2023
·Vol. 16
·期 11
·e202202379
·
IF 8.4
Peirong Lin,Yuheng Qi,Daying Guo,Xueyu Wang,Guoyong Fang,Xi'an Chen,Shun Wang
Graphical Mixing valences : The low-valence cobalt has better catalytic activity on polysulfides and improves the performance of the lithium-sulfur battery. Herein, we investigated in detail the effect of metal valences in different cobalt-based organic framework compounds on the kinetics of sulfur reaction in lithium-sulfur batteries (LSBs). On this basis, two organic framework compounds of zeolite-imidazole-based cobalt organic framework compound (Co-ZIF) and tetrakis(4-benzoic acid) porphyrinato-Co III chloride [Co-TBP(III)] with different valences were constructed as the functional intercalation separators of LSBs, and explored the effects of different valences on improving the reaction kinetics of polysulfides and inhibiting the shuttle effect. Experiments and theoretical calculations prove that Co II exhibits the best catalytic activity. This is mainly due to the fact that +2 valence shows a strong adsorption energy for polysulfides and a higher Fermi level compared with +3 valence, thus improving the efficiency of the rapid catalytic conversion of sulfur species. As expected, the discharge specific capacity of Co-ZIF as the catalytic layer of the LSBs reached 772.7 mAh g −1 at a high current density of 5 C. More importantly, the initial specific capacity is 839.6 mAh g −1 at high current 3 C, and after 720 cycles, the attenuation rate of per cycle is only 0.092 %, and the coulombic efficiency remains above 92 %.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
iScience
·
2023
·
IF 5.8
Jian Du,Yunxuan Ding,Yu Guo,Licheng Sun,Fei Li
Carbon-supported iron-cobalt bimetallic electrocatalysts usually exhibit robust catalytic activity toward the oxygen evolution reaction (OER). However, the spatial isolation of Fe species at atomic level on cobalt-carbon solid remains a great challenge for practical catalytic applications in the OER. Here, we report the fabrication of CoFe bimetal porous carbon electrocatalysts by pyrolysis of molecularly defined iron complexes such as FePc (Pc = phthalocyanine) and Fe(acac) 3 pre-encapsulated in the cavities of zeolitic imidazolate framework (ZIF)-67. With this unique strategy, high-loading atomic Fe nanoclusters (Fe-ACs) and Fe single atoms (Fe-SAs) were supported on Co/NC hybrids relying on the size of the molecular Fe precursors. The former exhibited superior OER performance to the single Fe atom-decorated Co/NC, as well as other ZIF-67-derived electrocatalysts. Theoretical modulation suggests Co as the OER active site for Fe-ACs@Co/NC at the in situ -formed FeOOH-ACs/Co 3 O 4 interface, while Fe was proposed as the active site for Fe-SAs@Co/NC.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Li Xu,Daijie Deng,Yuhui Tian,Hongping Li,Junchao Qian,Jianchun Wu,Henan Li
The sluggish kinetics of oxygen reduction reaction (ORR) is the bottleneck for practical applications of zinc-air batteries (ZABs). Developing highly efficient ORR electrocatalysts is of the essence for large-scale applications of ZABs. Herein, we design and synthesize the CoN x /Zn, N co-doped porous carbon structure (CoN x /Zn-NC) by self-polymerization of biomass materials and coupling of nitrogen-rich species with metallic ions. The introduced zinc element can regulate electronic structures of electrocatalysts and construct bimetallic active sites (N-Co/N-Zn species), facilitating the adsorption of reaction intermediates and further enhancing electrocatalytic performance. The porous carbon structure obtained by the self-polymerization of locust bean gum not only disperses active sites but also improves the O 2 and electron transfer efficiency of electrocatalysts. The CoN x /Zn-NC exhibited excellent ORR electrocatalytic performance (E 1/2 = 0.85 V) as well as outstanding stability. Impressively, the ZABs assembled with CoN x /Zn-NC demonstrated a high maximum power density, specific capacitance, and excellent charge/discharge cycling stability for 115 h, surpassing Pt/C catalyst.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Wenzheng Chen,Xuezhang Xiao,Jiahuan He,Zhong Dong,Xuancheng Wang,Man Chen,Lixin Chen
Sodium borohydride has attracted much attention because of its high hydrogen density, low hydrolysis temperature and safety. However, most of the current catalysts are expensive and their performances are easily attenuated. Therefore, the development of new catalysts with excellent performances and low cost is the key to its application. In this work, a novel dandelion-like CoMoNi–B/ZIF-67 catalyst with excellent performance was prepared by chemical reduction at room temperature, wherein the CoMoNi–B amorphous alloy was evenly wrapped on the ZIF-67 carrier through liquid phase reduction to form a dandelion-like composite catalyst, of which the “flower bud” ZIF-67 carrier is about 500 nm, and the “crown” flocculent amorphous alloy is about 400 nm. The as-synthesized CoMoNi–B/ZIF-67 has a dandelion-like structure, uniform distribution, large specific surface area, and exhibits an excellent catalytic activity with an apparent activation energy of 35.01 kJ/mol calculated by the Arrhenius equation . Its catalytic hydrolysis rate for sodium borohydride reaches up to 6277 (mL H 2 min/g Co and Ni) at 25 °C. Compared with traditional precious metal catalysts, this novel dandelion-like CoMoNi–B/ZIF-67 catalyst has simple preparation, low cost, and easy availability of raw materials, has great potential application for hydrogen generation in NaBH 4 hydrolysis.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jinxiu Zhao,Xuejing Liu,Xiang Ren,Bing Du,Xuan Kuang,Dongxu Tian,Qin Wei,Dan Wu
Highly efficient catalysts are required to solve the intrinsically sluggish kinetics of oxygen evolution reaction (OER). Herein, chromium doped cobalt carbonate hydroxide nanowire array on Ni foam (Cr-CoCH/NF) has been synthesized for the enhancement of OER activity and stability. Compared with pure CoCH/NF, Cr 0.2 -CoCH/NF, the optimal doping of Cr, shows a low overpotential of 203 mV at the current density of 10 mA cm −2 and a small Tafel slope of 84 mV dec −1 in 1.0 M NaOH. In addition, there is little deterioration in electrocatalytic performance after 1000-cycle cyclic voltammetry and the high activity can be maintained over 25 h. Density functional theory calculations reveal the Cr doping can regulate the electronic structure of nearby Co active center to achieve great enhancement of OER activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xuan Luo,Ruiying Zhu,Li Zhao,Xiaobo Gong
Tetracycline hydrochloride (TC) is one of the organic pollutants that can be consistently monitored in the aquatic environment and pose a great threat to the environment. The development of a bifunctional electro-Fenton (EF) catalyst capable of in situ H 2 O 2 production and decomposition to ·OH to degrade the pollutant is an efficient and green approach to deal with antibiotic pollution. The bifunctional catalysts Co, N double doped defective carbon materials were prepared by pyrolysis ball milling method using zeolite imidazolium ester skeleton structural materials (ZIFs) series materials as precursors, which showed more than 80% selectivity to H 2 O 2 and could basically remove TC within 120 min in EF system. Carbon defects and graphitic nitrogen can effectively improve the selectivity and yield of H 2 O 2 , while graphitization degree improves the charge transfer rate, the doping of Co and pyridinic-N contribute to the decomposition of H 2 O 2 into ·OH. The active species present in the Co 1 /Zn 1 -NPC/EF system is ·OH, and factors such as coexisting ions, humic acid and water quality have little effect on the efficiency of the degradation of TC in the Co 1 /Zn 1 -NPC/EF system, whereas Co 1 /Zn 1 -NPC electrocatalytic catalyst has excellent stability and stable treatment performance for a wide range of pollutants, as well as being an environmentally friendly green catalyst without metal leaching. Furthermore, the possible pathways and the toxicity hazard of TC degradation were proposed. The bifunctional electrocatalyst prepared in this research provides a novel strategy for the green and efficient treatment of pollutants in wastewater.
研究领域:
环境科学
·
催化材料
·
废水处理
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Danfeng Deng,Wenjing Song,Weizuo Li,Qiang Li,Xin Wang
A composite metal-organic frameworks (MOFs) structure, designated as Co-hmta@La-salen, was synthesized through coordination interactions between a one-dimensional lanthanum MOFs (La-salen) with high density of uncoordinated imine (–CH=N–) groups and a cobalt-based MOFs (Co-hmta) structure prepared using hydrogen bonding stacking with hexamethylenetetramine (hmta) as the organic ligand. Subsequently, the Co-hmta@La-salen composite was chosen as a template for the pyrolysis process to synthesize a La(OH) 3 supported metallic Co catalyst incorporating carbon-nitrogen (Co/La(OH) 3 -CN-hmta) catalyst. The catalytic results show that Co/La(OH) 3 -CN-hmta (54% and 46% selectivity for aniline and N-phenylbenzylamine, respectively) displays superior cascade performance compared to classic Co/La(OH) 3 -CN-nit catalyst (69% and 31% selectivity for aniline and N-phenylbenzylamine, respectively). Moreover, the kinetic test results indicate that N-alkylation is the rate-limiting step of the overall cascade reaction. The Co/La(OH) 3 -CN-hmta catalyst can be separated from the reaction system using a magnet, and it also exhibits good cyclic stability. All of these suggest that the “MOFs plus MOFs via coordination” templating method can be employed as an efficient strategy for the preparation of supported catalysts.
研究领域:
化学
·
催化材料科学
✓ 已验证
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 21
·4989
·
IF 4.2
Siyu Yue,Mengqi Tuo,Yemeng Sheng,Xinyu Guo,Jiufu Lu,Dong Wang
The solvothermal reactions involving cobalt ions with 5-methylisophthalic acid (H2MIP) and 1,3-bis(2-methylimidazol)propane (BMIP) yielded two cobalt(II) organic frameworks: {[Co4(MIP)4(BMIP)3]·1/2DMA}n(SNUT-31) and {[Co4(MIP)4(BMIP)3]·(EtOH)2·H2O]}n(SNUT-32) where DMA represents N,N-dimethylacetamide and EtOH signifies ethyl alcohol. Single-crystal X-ray diffraction analyses reveal thatSNUT-31andSNUT-32possess an isomorphic structure, featuring a unique 2-fold interpenetration of 3D frameworks in a parallel manner. Notably, bothSNUT-31andSNUT-32demonstrate remarkable performance in electrocatalytic oxygen evolution reactions and exhibit exceptional photocatalytic degradation capabilities against a model comprising three distinct dyes: rhodamine B, methyl orange, and methyl blue.
研究领域:
材料科学
·
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lifan Wang,Danya Gong,Siheng Niu,Leiying Wang,Qinling Shi,Xindong Wang,Jinli Qiao,Guicheng Liu,Chun Zhan
Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP)-based all-solid-state lithium battery (ASSLB) assembled with Ni-rich layered cathode (NCM), of much interest because of its high energy–density and safety, presents many challenges, one of which is poor interfacial instability resulting in large interfacial resistance. Nevertheless, the mechanism of electrochemical side reactions on the interfacial deterioration hasn’t been much investigated specifically, despite their close relationships in electrochemical performance. Herein, we report that the fundamental origin of interfacial chemical reactions is the migration of Ni 2+ from the nickel-rich cathodes to the NCM/LATP interface, for the first time, and the simultaneous chemical reaction with Ti 4+ in LATP, followed by the decomposition of LATP. In view of this, an elaborately designed regulation strategy, in-situ construction of the layered perovskite La 4 NiLiO 8 buffer layer , is proposed to effectively reduce the content of Ni 2+ on the surface of the nickel-rich cathodes and alleviate the chemical reaction between Ni 2+ and Ti 4+ , thereby improving the interfacial stability between NCM and LATP. As a result, the assembled ASSLBs with the La 4 NiLiO 8 buffer layer exhibit high initial discharge capacity (171.49 mAh/g) and excellent cycling performance with 89.47 % capacity retention after 100 cycles at 0.1C.
研究领域:
材料科学
·
电化学
·
能源存储技术
✓ 已验证
DOI
高影响因子
Materials Chemistry Frontiers
·
2017
·Vol. 1
·期 10
·2065-2077
·
IF 0
Fu Yang,Bangbang Wang,Hang Su,Shijian Zhou,Yan Kong
Surface defective or heterojunction sites of catalysts generally afford remarkable catalytic activity thanks to their high-surface-energy. Regularly-generating multiple defective sites on the surface of a catalyst is exceedingly promising in many reactions. In this study, we report an unexpected Co/Fe–Co planar hybrid composite nanosheet with serried surface defects including surface biphasic junction sites or defective holes. A facile thermal-induced process was applied to trigger the generation of defective sites on planar Co/Fe–Co hydroxides. Through a controlled thermal process, massive serried CoO nanocrystals were in situ dissolved out of the surface of cobalt hydroxide, while defective surface holes were formed on the Fe-doped Co(OH)2 nanosheets under a prolonged thermal procedure. The morphology and microscale structure of the resulting Co/Fe–Co hybrid 2-dimensional (2D) composites were systematically examined by virtue of various characterization techniques. As expected, the obtained surface defective Co/Fe–Co planar composites showed obviously enhanced catalytic activity in the Fenton-like reaction. Based on a catalytic study, we proved that the CoO nanocrystals densely-distributed on thinlayer Co(OH)2. Uniformly-introduced Fe heteroatoms in the inter-structure of Co(OH)2, along with the formed surface defective holes on Fe–Co hybrid composites, are synergistically responsible for increased catalytic removal efficiency of MB in the presence of peroxomonosulfate.
研究领域:
无机化学
·
催化化学
·
纳米材料科学
·
环境化学
·
物理化学
✓ 已验证
DOI
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Wei Wang,Wenhua Cheng,Zhenjie Liu,Murong Xi,Zhouliang Tan,Yadong Wang,Weilu Zhang,Pingping Chang,Zihan Qi,Huan Zhou,Han Zhang,Juan Ding,Yudai Huang
The commercialization of Ni-rich layered oxide cathode materials has been severely hampered by rapid capacity degradation and safety issues. Here, we demonstrate a lattice reconstruction strategy to improve the structural and thermal stability of LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM83) via calcium. The enhanced stability of NCM83 is ascribed to the formation of Ca-O bond, which is stronger than TM-O (TM=Ni, Mn, Co) bond. The lattice reconstruction enables metal-O (M-O) bond more stable which mitigates the loss of lattice oxygen, thus improving the reversibility of the H2-H3 phase transition in NCM83. Moreover, Ca 2+ acts as a pillar, facilitating the transport of Li + . The lattice-reconstructed Ni-rich cathode material with 0.5 % Ca can maintain a capacity retention ratio of 97.3 % at 1 C after 150 cycles. As compared with the pristine NCM83 cathode, the high-voltage cycling stability at 4.5 V and high-temperature performance at 55 °C are increased by 17.9 % and 12.2 %, respectively. This work actually proposes a new approach to design and construct high-performance Ni-rich cathode materials for practical lithium-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ximin Ling,Wutao Wei,Changwei Shan,Xuyan Qin,Mingjie Song,Zhao Liu,Liwei Mi
Mg 2+ /Li + hybrid batteries (MLHBs), which support the rapid insertion and removal of Mg 2+ /Li + bimetallic ions, are promising energy storage systems. Inspired by the Kirkendall effect, ball-in-ball bimetallic sulfides with heterostructures were prepared as cathode materials for the MLHBs. First, a nickel–cobalt precursor (NiCo-X precursor) with three-dimensional (3D) nanosheets on its surface was prepared using a solvothermal method based on the association reaction between alkoxide molecules. Subsequently, the NiCo-X precursor was vulcanized at high temperature using the potential energy difference as the driving force to successfully prepare NiS 2 @CoS 2 core–shell hollow spheres. When used as the positive electrode material for the MLHBs, the NiS 2 @CoS 2 hollow spheres exhibited excellent Mg 2+ /Li + ion storage capacity, high specific capacity, good rate performance, and stable cyclic stability owing to their tough hierarchical structure. At a current density of 500 mA g −1 , a specific capacity of 536 mAh g −1 was maintained after 200 cycles. By explaining the transformation mechanism of Mg 2+ /Li + in bimetallic sulfides, it was proven that Mg 2+ and Li + worked cooperatively. This study provides a new approach for developing MLHBs with good electrochemical properties.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）