A General Approach to Shaped MOF‐Containing Aerogels toward Practical Water Treatment Application

Cheng, Puxin; Kim, Minjun; Lim, Hyunsoo; Lin, Jianjian; Torad, Nagy L.; Zhang, Xiaogang; Hossain, Md. Shahriar A.; Wu, Chia-Wen; Wang, Chaohai; Na, Jongbeom; Yamauchi, Yusuke

doi:10.1002/adsu.202000060

Cited by 49 publications

(26 citation statements)

References 36 publications

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“…The development of advanced materials for renewable energy applications has attracted increasing research attention in recent years [1][2][3][4]. As an abundant, zero carbon emission source and renewable energy carrier, hydrogen plays an important role in sustainable energy and industrial chemical systems [5][6][7][8]. Hydrogen production through electrochemical water-splitting is a type of hydrogen-production technology that is advantageous owing to its high energy-conversion rate and environmentally friendly process [9][10][11][12][13].…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution

et al. 2021

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The hydrogen evolution reaction (HER) through electrocatalysis is promising for the production of clean hydrogen fuel. However, designing the structure of catalysts, controlling their electronic properties, and manipulating their catalytic sites are a significant challenge in this field. Here, we propose an electrochemical surface restructuring strategy to design synergistically interactive phosphorus-doped carbon@MoP electrocatalysts for the HER. A simple electrochemical cycling method is developed to tune the thickness of the carbon layers that cover on MoP core, which significantly influences HER performance. Experimental investigations and theoretical calculations indicate that the inactive surface carbon layers can be removed through electrochemical cycling, leading to a close bond between the MoP and a few layers of coated graphene. The electrons donated by the MoP core enhance the adhesion and electronegativity of the carbon layers; the negatively charged carbon layers act as an active surface. The electrochemically induced optimization of the surface/interface electronic structures in the electrocatalysts significantly promotes the HER. Using this strategy endows the catalyst with excellent activity in terms of the HER in both acidic and alkaline environments (current density of 10 mA cm−2 at low overpotentials, of 68 mV in 0.5 M H2SO4 and 67 mV in 1.0 M KOH).

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Section: Introductionmentioning

confidence: 99%

Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution

et al. 2021

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“…Adsorption of anionic dye MO, selectivity toward MO from an anionic/cationic dye mixture of MO/MB [111] Direct mixing 3D aerogel UiO-66-NH 2 -CS aerogel monolith (UNCAM) Adsorption of Pb(II) [112] In situ growth 3D aerogel Ni/Co-MOF@CMC aerogels Adsorption of tetracycline hydrochloride and bacteriostatic agent [113] Direct mixing 3D aerogel UiO-66/cellulose aerogels Adsorption of MB and MO [114] Direct mixing 3D aerogel ZIF-8 (ZIF-67)/AG aerogel Adsorption of RhB [115] Direct mixing 3D Carbon gel 3D porous carbon monolith (PZ-2-C) Adsorption of MB and MO [116] Tremendous efforts have been undertaken to seek feasible methods and synthesis strategies and applications in water treatment of typical MOF-based macroscopic materials are summarized in Table 1. [17,[98][99][100][101][102][103][104][105][106][107][108][109][110][111][112][113][114][115][116] These catalysts can simplify the process of water treatment, improve water treatment capacity, and avoid the secondary pollution caused by powder MOF.…”

Section: Discussionmentioning

confidence: 99%

Macroscopic MOF Architectures: Effective Strategies for Practical Application in Water Treatment

Yao

Wang

et al. 2021

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Metal–organic frameworks (MOFs) have potential applications in removing pollutants such as heavy metals, oils, and toxins from water. However, due to the intrinsic fragility of MOFs and their fine powder form, there are still technical barriers to their practical application such as blockage of pipes, difficulty in recovery, and potential environmental toxicity. Therefore, attention has focused on approaches to convert nanocrystalline MOFs into macroscopic materials to overcome these limitations. Recently, strategies for shaping MOFs into beads (0D), nanofibers (1D), membranes (2D), and gels/sponges (3D) with macrostructures are developed including direct mixing, in situ growth, or deposition of MOFs with polymers, cotton, foams or other porous substrates. In this review, successful strategies for the fabrication of macroscopic materials from MOFs and their applications in removing pollutants from water including adsorption, separation, and advanced oxidation processes, are discussed. The relationship between the macroscopic performance and the microstructure of materials, and how the range of 0D to 3D macroscopic materials can be used for water treatment are also outlined.

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“…Metal–organic frameworks (MOFs) are crystalline coordination networks composed of a metal cation or cluster nodes and organic linkers which form porous structures. − Physical and chemical tunability, high surface area, and well-defined structural geometry make MOFs interesting materials for study as heterogeneous catalysts. − However, for many catalytic MOF systems, the pore aperture s of MOFs can be too narrow to allow for facile substrate diffusion into channels to access intrapore metal sites, limiting catalytic activity to metal sites on (or extremely close to) the external surfaces of MOF particles. − …”

Section: Introductionmentioning

confidence: 99%

Cu-Based Metal–Organic Framework Nanosheets Synthesized via a Three-Layer Bottom-Up Method for the Catalytic Conversion of S-Nitrosoglutathione to Nitric Oxide

Thai

Tuttle

DeRoo

et al. 2021

ACS Appl. Nano Mater.

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Metal–organic framework nanosheets (MOFNs) are promising materials for heterogeneous catalysis systems where active metal sites are positioned on particle exterior surfaces. The hypothesis that intrapore metal sites are active for catalysis has been disproven for certain systems, and therefore the synthesis of MOF particles with increased external surface area and density of metal active sites is needed. MOFNs provide an increased proportion of metal sites accessible to substrates that experience limited or no diffusion into MOF pores compared to MOF particles with other morphologies such as octahedra. However, developing synthetic methods to generate a variety of MOFNs remains an experimental challenge, particularly for water-stable materials. Herein, we use a three-layer method to synthesize the nanosheet particles of a new MOF, CuBDTri (where H2BDTri = 1,4-di(1H-1,2,3-triazol-5-yl)benzene). Scanning electron microscopy (SEM), powder X-ray diffraction (pXRD), Brunauer–Emmett–Teller (BET) analysis, inductively coupled plasma atomic emission spectroscopy (ICP-AES), and acid digestion with time-of-flight mass spectrometry (TOF-MS) were used to characterize the newly synthesized CuBDTri nanosheets. Both the synthetic method and linker identity were shown to impact the anisotropic growth of MOF particles with nanosheet morphologies. Importantly, this is the first report of using the three-layer method to synthesize MOFNs with Cu–N linkages, meaning that the three-layer method is (i) more broadly applicable than previously known (having only been used previously to synthesize nanosheets with Cu-oxo linkages) and (ii) can be used to synthesize water-stable Cu-MOFNs in situ (a key result, given MOFs with Cu-oxo linkages usually exhibit poor water stability). CuBDTri nanosheets are also more catalytically active on a per-total-Cu-atom basis for a standardized test reaction (nitric oxide (NO) generation from S-nitrosoglutathione (GSNO)) than previously studied octahedral particles of the MOF CuBTTri (where H3BTTri = 1,3,5-tris(1H-1,2,3-triazol-5-yl)benzene), supporting the hypothesis that MOFNs are superior to particles with other morphologies for reactions where catalytic activity is limited to particle exterior surfaces (such as the NO generation reaction).

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A General Approach to Shaped MOF‐Containing Aerogels toward Practical Water Treatment Application

Cited by 49 publications

References 36 publications

Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution

Electrochemical Surface Restructuring of Phosphorus-Doped Carbon@MoP Electrocatalysts for Hydrogen Evolution

Macroscopic MOF Architectures: Effective Strategies for Practical Application in Water Treatment

Cu-Based Metal–Organic Framework Nanosheets Synthesized via a Three-Layer Bottom-Up Method for the Catalytic Conversion of S-Nitrosoglutathione to Nitric Oxide

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