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185 results on '"Chen, Shixia"'

13. Topology Reconfiguration of Anion‐Pillared Metal‐Organic Framework from Flexibility to Rigidity for Enhanced Acetylene Separation

Author

Xiong, Hanting, primary, Peng, Yong, additional, Liu, Xing, additional, Wang, Pengxiang, additional, Zhang, Peixin, additional, Yang, Longsheng, additional, Liu, Junhui, additional, Shuai, Hua, additional, Wang, Lingmin, additional, Deng, Zhenning, additional, Chen, Shixia, additional, Chen, Jingwen, additional, Zhou, Zhenyu, additional, Deng, Shuguang, additional, and Wang, Jun, additional

Published
2024
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26. In situ transformation of a Bi-based MOF to a highly active catalyst for CO2 reduction.

Author

Liu, Chan, Wu, Zeliang, Li, Yuhan, Yu, Haoming, Chen, Shixia, Hong, Wei, Deng, Shuguang, and Wang, Jun

Subjects
CARBON dioxide reduction, ELECTROCATALYSIS, CATALYSTS, ELECTROLYTIC reduction, METAL-organic frameworks, CARBON cycle, FORMIC acid
Abstract

Electrochemical carbon dioxide reduction reaction (ECO2RR) is an effective means to promote carbon cycling. Recently, Bi-based metal–organic frameworks (MOFs) have attracted significant attention due to their high efficiency for formic acid generation in ECO2RR, however, their composition and morphology transformation during electrocatalysis still lack a deep exploration. Herein, a Bi-MOF with 2,4,6-tris(4-carboxyphenyl)-1,3,5-triazine (H3TATB) ligand is used as the prototype to investigate its in situ transformation during ECO2RR. With various characterization methods, the detailed transformation processes are revealed. Firstly, the Bi-MOF was transformed into Bi2O2CO3 due to ligand substitution in KHCO3 electrolyte, resulting in changes in both shape and composition. Secondly, during ECO2RR, the Bi3+ ions can be reduced into metallic Bi0 nanoparticles and act as the real active component for ECO2RR. The resultant catalyst exhibits a high selectivity of up to 94.3% towards formate generation. At an optimal potential of −1.08 V vs. RHE, the catalyst can maintain a current density of −25 mA cm−2 and a faradaic efficiency of formate over 90% for 14.5 hours. This work not only develops an efficient electrocatalyst for ECO2RR but also provides a new insight into the in situ reconstruction of MOF precursor into the active catalyst, which is useful for the design and synthesis of other materials. [ABSTRACT FROM AUTHOR]

Published
2024
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37. Electro‐field alignment in a novel metal–organic framework for benchmark separation of ethylene from a ternary gas mixture.

Author

Wang, Lingmin, Zhang, Yan, Zhang, Peixin, Liu, Xing, Xiong, Hanting, Krishna, Rajamani, Liu, Junhui, Shuai, Hua, Wang, Pengxiang, Zhou, Zhenyu, Chen, Jingwen, Chen, Shixia, Deng, Shuguang, and Wang, Jun

Subjects
METAL-organic frameworks, ETHYLENE, CARBON dioxide, ADSORPTIVE separation, ADSORPTION capacity, GAS mixtures
Abstract

One‐step separation of C2H4 from ternary gas mixtures containing acetylene (C2H2), ethylene (C2H4), and carbon dioxide (CO2) represents a great challenge in chemical industry. Herein, we report the electro‐field alignment in a novel anion‐pillared MOF (SIFSIX‐TEPE‐Cu) for benchmark C2H4 separation from C2H2/CO2/C2H4 gas mixtures. The semi‐cage cavities featuring capped facets generated negative potentials along anion pillars and compensatory positive‐charged electro‐fields along organic ligands (TEPE) that facilitate specific recognitions of C2H2 and CO2 over C2H4. As a result, SIFSIX‐TEPE‐Cu exhibits high adsorption capacities for C2H2 (123 cm3 g−1) and CO2 (65 cm3 g−1) at 1.0 bar and 298 K. Notably, the record‐high C2H2 uptake (78 cm3 g−1) at 0.01 bar and remarkable C2H2/C2H4 selectivity (615.2) renders benchmark trace C2H2 removal ability. Dynamic breakthrough experiments demonstrate the benchmark productivity for high‐purity C2H4 (>99.995%) of 194.7 mol kg−1 and 5.96 mol kg−1 from binary C2H2/C2H4 (1/99, v/v) and ternary C2H2/CO2/C2H4 (1/9/90, v/v/v) gas mixtures. [ABSTRACT FROM AUTHOR]

Published
2024
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41. In SituReconstruction of Scalable Amorphous Indium-Based Metal–Organic Framework for CO2Electroreduction to Formate over an Ultrawide Potential Window

Author

Liu, Ziyun, Han, Xinxin, Liu, Junhui, Chen, Shixia, Deng, Shuguang, and Wang, Jun

Abstract

Amorphous metal–organic frameworks (aMOFs) are highly attractive for electrocatalytic applications due to their exceptional conductivity and abundant defect sites, but harsh preparation conditions of “top-down” strategy have hindered their widespread use. Herein, the scalable production of aMIL-68(In)-NH2was successfully achieved through a facile “bottom-up” strategy involving ligand competition with 2-methylimidazole. Multiple in situand ex situcharacterizations reveal that aMIL-68(In)-NH2evolutes into In/In2O3–xas the genuine active sites during the CO2electrocatalytic reduction (CO2RR) process. Moreover, the retained amino groups could enhance the CO2adsorption. As expected, the reconstructed catalyst demonstrates high formate Faradaic efficiency values (>90%) over a wide potential range of 800 mV in a flow cell, surpassing most top-ranking electrocatalysts. Density functional theory calculations reveal that the abundant oxygen vacancies in aMIL-68(In)-NH2induce more local charges around electroactive sites, thereby promoting the formation of HCOO* intermediates. Furthermore, 16 g of samples can be readily prepared in one batch and exhibit almost identical CO2RR performances. This work offers a feasible batch-scale strategy to design amorphous MOFs for the highly efficient electrolytic CO2RR.

Published
2024
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43. Interaction-selective molecular sieving adsorbent for direct separation of ethylene from senary C2-C4 olefin/paraffin mixture.

Author

Peng, Yong, Xiong, Hanting, Zhang, Peixin, Zhao, Zhiwei, Liu, Xing, Tang, Shihui, Liu, Yuan, Zhu, Zhenliang, Zhou, Weizhen, Deng, Zhenning, Liu, Junhui, Zhong, Yao, Wu, Zeliang, Chen, Jingwen, Zhou, Zhenyu, Chen, Shixia, Deng, Shuguang, and Wang, Jun

Subjects
ALKENES, MOLECULAR sieves, PARAFFIN wax, ADSORPTIVE separation, ETHYLENE, VINYL acetate, ALKANES, METALLOCENE catalysts
Abstract

Olefin/paraffin separations are among the most energy-intensive processes in the petrochemical industry, with ethylene being the most widely consumed chemical feedstock. Adsorptive separation utilizing molecular sieving adsorbents can optimize energy efficiency, whereas the size-exclusive mechanism alone cannot achieve multiple olefin/paraffin sieving in a single adsorbent. Herein, an unprecedented sieving adsorbent, BFFOUR-Cu-dpds (BFFOUR = BF4-, dpds = 4,4'-bipyridinedisulfide), is reported for simultaneous sieving of C2-C4 olefins from their corresponding paraffins. The interlayer spaces can be selectively opened through stronger guest-host interactions induced by unsaturated C = C bonds in olefins, as opposed to saturated paraffins. In equimolar six-component breakthrough experiments (C2H4/C2H6/C3H6/C3H8/n-C4H8/n-C4H10), BFFOUR-Cu-dpds can simultaneously divide olefins from paraffins in the first column, while high-purity ethylene (> 99.99%) can be directly obtained through the subsequent column using granular porous carbons. Moreover, gas-loaded single-crystal analysis, in-situ infrared spectroscopy measurements, and computational simulations demonstrate the accommodation patterns, interaction bonds, and energy pathways for olefin/paraffin separations. Olefin/paraffin separations are challenging in chemical industry. Here, authors report a sieving adsorbent for separating C2-C4 olefins from counterpart paraffins. The interlayer spaces are selectively opened via stronger guest-host interactions induced by olefins, as opposed to saturated paraffins. [ABSTRACT FROM AUTHOR]

Published
2024
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46. Enhancing electrocatalytic N2reduction to NH3by introducing Ni heteroatoms into NiCuOxelectrocatalystElectronic supplementary information (ESI) available. See DOI: https://doi.org/10.1039/d4cy00482e

Author

Han, Xinxin, Zhou, Weizhen, Huang, Xin, Yu, Haoming, Yang, Fangqi, Chen, Shixia, and Wang, Jun

Abstract

Modulating the local electronic structure in 3d transition metal oxides is appealing in the N2reduction reaction (NRR), yet remains challenging. Herein, Ni dopants with higher electronegativity are introduced to tune the electronic density of Cu in flower-like NiCuOxthrough low-temperature calcination of the readily formed NiCu(OH)xprecursor. The as-obtained catalyst delivers a remarkable NH3production of 11.78 μg h−1mgcat.–1with a high faradaic efficiency of 19.28% at a low voltage of −0.2 V, superior to most NRR electrocatalysts at similar voltages. XPS, in situRaman, and DFT calculation reveal that the Ni dopant enhances the local electronic density surrounding Cu sites, which is favorable for reducing the energy barrier of the rate-determining (*N2to *NNH) step of the NRR as well as depressing the competing hydrogen evolution reaction. This work provides new insight into the effect of hetero-metal-atom doping on the NRR process and is instructive for the rational design of high-performance electrocatalysts.

Published
2024
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47. Engineering Pore Environments of Sulfate‐pillared Metal‐Organic Framework for Efficient C 2 H 2 /CO 2 Separation with Record Selectivity

Author

Liu, Xing, primary, Zhang, Peixin, additional, Xiong, Hanting, additional, Zhang, Yan, additional, Wu, Ke, additional, Liu, Junhui, additional, Krishna, Rajamani, additional, Chen, Jingwen, additional, Chen, Shixia, additional, Zeng, Zheling, additional, Deng, Shuguang, additional, and Wang, Jun, additional

Published
2023
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