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6. Reticular chemistry guided precise construction of zirconium-pentacarboxylate frameworks with 5-connected Zr6 clusters

Author

Peng, Tianyou, primary, Han, Chao-Qin, additional, Xia, Hai-Lun, additional, Zhou, Kang, additional, Zhang, Jian, additional, Si, Jincheng, additional, Wang, Lei, additional, Miao, Jiafeng, additional, Guo, Fu-An, additional, Wang, Hao, additional, Qu, Lu-Lu, additional, Xu, Guozhong, additional, Li, Jing, additional, and Liu, Xiao-Yuan, additional

Published
2024
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18. Electrochemically exfoliated Ni-doped MoS2nanosheets for highly efficient hydrogen evolution and Zn-H2O battery

Author

Wei, Hao, Si, Jincheng, Zeng, Libin, Lyu, Siliu, Zhang, Zhiguo, Suo, Yange, and Hou, Yang

Abstract

Thanks to tunable physical and chemical properties, two-dimensional (2D) materials have received intensive interest, endowing their excellent electrocatalytic performances for applications in energy conversion. However, their catalytic activities are largely determined by poor adsorption energy and limited active edge sites. Herein, a one-step electrochemical exfoliation strategy was developed to fabricate 2D Ni-doped MoS2nanosheets (Ni-EX-MoS2) with a lateral size of ∼500 nm and thickness of ∼3.5 nm. Profiting from high electrical conductivity and abundant exposing active sites, Ni-EX-MoS2catalyst displayed an admirable performance for electrochemical hydrogen evolution reaction (HER) with a low overpotential of 145 mV at 10 mA/cm2as well as a small Tafel slope of 89 mV/dec in alkaline media, which are superior to those of the most reported MoS2-based electrocatalysts. The formed Ni species with tuning electronic structure played a crucial role as primary active center of Ni-EX-MoS2, as well as the forming stable 1T/2H phase MoS2interface demonstrated a synergistic effect on electrocatalytic HER performance. Further, Ni-EX-MoS2was employed as a cathode electrode for alkaline Zn-H2O battery, which displayed a high power density of 3.3 mW/cm2with excellent stability. This work will provide a simple and effective guideline for design of electrochemically exfoliated transition metal-doped MoS2nanosheets to inspire their practical applications in energy catalytic and storage.

Published
2023
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19. Reticular chemistry guided precise construction of zirconium-pentacarboxylate frameworks with 5-connected Zr 6 clusters.

Author

Peng T, Han CQ, Xia HL, Zhou K, Zhang J, Si J, Wang L, Miao J, Guo FA, Wang H, Qu LL, Xu G, Li J, and Liu XY

Abstract

Zirconium-based metal-organic frameworks (Zr-MOFs) have been extensively studied due to their very rich structural chemistry. The combination of nearly unlimited carboxylic acid-based linkers and Zr 6 clusters with multiple connectivities has led to diverse structures and specific properties of resultant Zr-MOFs. Herein, we demonstrate the successful use of reticular chemistry to construct two novel Zr-MOFs, HIAM-4040 and HIAM-4040-OH, with zfu topology. Based on a thorough structural analysis of (4,4)-connected lvt-type Zr-tetracarboxylate frameworks and a judicious linker design, we have obtained the first example of a Zr-pentacarboxylate framework featuring unprecedented 5-connected organic linkers and 5-connected Zr 6 clusters. Compared with HIAM-4040, a larger Stokes shift is achieved in HIAM-4040-OH via hydroxyl group induced excited-state intramolecular proton transfer (ESIPT). HIAM-4040-OH exhibits high chemical and thermal stability and is used for HClO detection in aqueous solution with excellent sensitivity and selectivity., Competing Interests: The authors declare no competing financial interests., (This journal is © The Royal Society of Chemistry.)

Published
2024
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20. Ultrathin tin monosulfide nanosheets with the exposed (001) plane for efficient electrocatalytic conversion of CO 2 into formate.

Author

Chen H, Chen J, Si J, Hou Y, Zheng Q, Yang B, Li Z, Gao L, Lei L, Wen Z, and Feng X

Abstract

Current Sn-based materials are ideal catalysts developed to drive the electrochemical conversion of CO 2 to formate, but competing proton reduction to hydrogen is an ever-present drain on catalytic selectivity. Herein, we report a reliable electrochemical exfoliation route, with the assistance of alternating voltage, for large-scale preparation of two-dimensional (2D) ultrathin tin monosulfide nanosheets (SnS NSs), which feature a large lateral size of 1.0 μm with a thickness of ∼5.0 nm. Systematic electrochemical studies demonstrated that the achieved SnS NSs exhibited an outstanding electrocatalytic activity towards the CO 2 reduction reaction (CO 2 RR) to the formate product, as evidenced by a considerable faradaic efficiency (F.E.) of 82.1%, a high partial current density of 18.9 mA cm -2 at -1.1 V, and a low Tafel slope of 180 mV dec -1 . Further, using an electrode prepared from the resulting SnS NSs by the particle transfer method, a remarkably high formate F.E. over 91% was achieved in a wide potential window. Such high performance renders the SnS NSs among the best reported tin sulfide-based CO 2 RR electrocatalysts. Theoretical calculations coupled with comprehensive experimental studies demonstrated that the synergistic effect between the ultrathin layered architecture and dominantly exposed (001) plane of SnS NSs accounted for the uniquely efficient catalytic activity for the CO 2 RR., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Published
2020
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