Ultrahigh-permeance functionalized boron nitride membrane for nanoconfined heterogeneous catalysis

Asif, Muhammad Bilal; Zhang, Shaoze; Qiu, Ling; Zhang, Zhenghua

doi:10.1016/j.checat.2022.01.003

Cited by 30 publications

(20 citation statements)

References 45 publications

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“…In h-BN-derived nanocatalysts, boron or nitrogen sites with unsaturated coordination that form at the edge position or within the defects could directly act as the active sites to promote the reaction or provide the surrounding environment to tune the electronic properties of the active metal center (e.g., supported metal nanoparticles (NPs) or single atoms (SAs)) toward enhanced catalytic activity. − Under either circumstance, the electronic and structural properties of h-BN play critical roles, which could be modulated by the number of 2D layers, defect types and ratios, crystallinity, surface functionalization, and heteroelemental doping. , Therefore, the development of facile and controllable construction and modification approaches is a prerequisite to accessing the precise tuning over the h-BN scaffolds, which will, in turn, become powerful platforms for generating heterogeneous catalysts with promising catalytic performance. In addition, a fundamental and systematic understanding of the correlation between specific structural and compositional parameters and the catalytic behavior variation, particularly the charge transfer and interfacial phenomena in h-BN-supported metal catalysts, will provide untapped opportunities in catalyst design and resolve challenging issues in catalysis by customizing the h-BN scaffolds.…”

Section: Introductionmentioning

confidence: 99%

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

et al. 2022

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Hexagonal boron nitrides (h-BNs) are attractive two-dimensional (2D) nanomaterials that consist of alternating B and N atoms and layered honeycomblike structures similar to graphene. They have exhibited unique properties and promising application potentials in the field of energy storage and transformation. Recent advances in utilizing h-BN as a metal-free catalyst in the oxidative dehydrogenation of propane have triggered broad interests in exploring h-BN in catalysis. However, h-BN-based materials as robust nanocatalysts in heterogeneous catalysis are still underexplored because of the limited methodologies capable of affording h-BN with controllable crystallinity, abundant porosity, high purity, and defect engineering, which played important roles in tuning their catalytic performance. In this Account, our recent progress in addressing the above issues will be highlighted, including the synthesis of high-quality h-BN-based nanomaterials via both bottom-up and top-down pathways and their catalytic utilization as metal-free catalysts or as supports to tune the interfacial electronic properties on the metal nanoparticles (NPs). First, we will focus on the large-scale fabrication of h-BN nanosheets (h-BNNSs) with high crystallinity, improved surface area, satisfactory purity, and tunable defects. h-BN derived from the traditional approaches using boron trioxide and urea as the starting materials generally contains carbon/oxygen impurities and has low crystallinity. Several new strategies were developed to address the issues. Using bulk h-BN as the precursor via gas exfoliation in liquid nitrogen, single-or few-layered h-BNNS with abundant defects could be generated. Amorphous h-BN precursors could be converted to h-BN nanosheets with high crystallinity assisted by a magnesium metallic flux via a successive dissolution/precipitation/crystallization procedure. The as-fabricated h-BNNS featured high crystallinity and purity as well as abundant porosity. An ionothermal metathesis procedure was developed using inorganic molten salts (NaNH 2 and NaBH 4 ) as the precursors. The h-BN scaffolds could be produced on a large scale with high yield, and the asafforded materials possessed high purity and crystallinity. Second, utilization of the as-prepared h-BN library as metal-free catalysts in dehydrogenation and hydrogenation reactions will be summarized, in which they exhibited enhanced catalytic activity over the counterparts from the previous synthesis method. Third, the interface modulation between metal NPs with the as-prepared defects' abundant h-BN support will be highlighted. The h-BN-based strong metal−support interaction (SMSI) nanocatalysts were constructed without involving reducible metal oxides via the ionothermal procedure we developed by deploying specific inorganic metal salts, acting as robust nanocatalysts in CO oxidation. Under conditions simulated for practical exhaust systems, promising catalytic efficiency together with high thermal stability and sintering resistance was achieved. Across all of these ...

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Section: Introductionmentioning

confidence: 99%

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

et al. 2022

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“…By confining catalytic reactions within a nanoscale space, the selectivity can be significantly enhanced and the reaction kinetics can be massively accelerated under mild process conditions [2][3][4] . Consequently, nanoconfinement catalysts with unique geometric and electronic structures have been developed to enhance the catalytic performance for water treatment [5][6][7][8][9] . For instance, Fe 2 O 3 nanoparticles (~2 nm) confined within multi-walled carbon nanotube (CNT) with an inner diameter of 7 nm show 22.5 times higher methylene blue degradation rates than without the CNT encapsulation 8 .…”

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confidence: 99%

Angstrom-confined catalytic water purification within Co-TiOx laminar membrane nanochannels

et al. 2022

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The freshwater scarcity and inadequate access to clean water globally have rallied tremendous efforts in developing robust technologies for water purification and decontamination, and heterogeneous catalysis is a highly-promising solution. Sub-nanometer-confined reaction is the ultimate frontier of catalytic chemistry, yet it is challenging to form the angstrom channels with distributed atomic catalytic centers within, and to match the internal mass transfer and the reactive species’ lifetimes. Here, we resolve these issues by applying the concept of the angstrom-confined catalytic water contaminant degradation to achieve unprecedented reaction rates within 4.6 Å channels of two-dimensional laminate membrane assembled from monolayer cobalt-doped titanium oxide nanosheets. The demonstrated degradation rate constant of the target pollutant ranitidine (1.06 ms−1) is 5–7 orders of magnitude faster compared with the state-of-the-art, achieving the 100% degradation over 100 h continuous operation. This approach is also ~100% effective against diverse water contaminates with a retention time of <30 ms, and the strategy developed can be also extended to other two-dimensional material-assembled membranes. This work paves the way towards the generic angstrom-confined catalysis and unravels the importance of utilizing angstrom-confinement strategy in the design of efficient catalysts for water purification.

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“…NPC, NPC-Co, PtCo/NPC, and PtCo/NPC-Co all exhibited typical III hysteresis loops (from 0.45 to 1.0) and IV isotherm behavior at low pressure (<0.05), indicating the presence of hierarchical porous features with the coexistence of micropores, mesopores, and macropores. , The Horvath–Kawazoe (HK) and Barrett–Joyner–Halenda (BJH) models were used to analyze the formation of pore structures in the supports. The BJH model is usually used to estimate the pores with particle size > 5 nm, while the HK model is commonly used to estimate the pores with a particle size <5 nm (including micropores). , The removal of Co metal with an average particle size of 3.9 nm after acid washing reduced the microporosity of NPC-Co (12.3%) by 25.4% compared with that of NPC (16.5%). Comparing the pore size distributions of NPC and NPC-Co (Figure a,b), the proportion of mesopores increases at approximately 3.9 nm, whereas the proportion of micropores decreases significantly, which can verify the aforementioned conjecture.…”

Section: Resultsmentioning

confidence: 99%

“…The BJH model is usually used to estimate the pores with particle size > 5 nm, while the HK model is commonly used to estimate the pores with a particle size <5 nm (including micropores). 46,47 The removal of Co metal with an average particle size of 3.9 nm after acid washing reduced the microporosity of NPC-Co (12.3%) by 25.4% compared with that of NPC (16.5%). Comparing the pore size distributions of NPC and NPC-Co (Figure 4a,b), the proportion of mesopores increases at approximately 3.9 nm, whereas the proportion of micropores decreases significantly, which can verify the aforementioned conjecture.…”

Section: Resultsmentioning

confidence: 99%

Nitrogen-Doped Porous Carbon-Supported PtCo Nanoparticle Electrocatalyst for Oxygen Reduction Reaction Prepared by a Dual-Template Method

Guo

Dai

et al. 2023

ACS Appl. Energy Mater.

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A strategy for preparing nitrogen-doped porous carbon (NPC-Co) using a dual-template method is reported in this study. The catalyst (PtCo/NPC-Co) with high catalytic performance for the oxygen reduction reaction (ORR) was developed after adding PtCo metal nanoparticles (NPs). Polydopamine can complex metals, encapsulate templates, and reduce metals. Therefore, polydopamine was selected as the carbon and nitrogen source. Then, ZnO and Co NPs were used as a double template to obtain a carrier (NPC-Co) with a high mesoporous ratio and high N content. The PtCo alloy NPs are homogeneously anchored on the support by highly dispersed N atoms originating from NPC-Co. PtCo/NPC-Co exhibited excellent catalytic performance and durability for oxygen reduction. The mass activity of PtCo/NPC-Co is 4.8 times that of commercial Pt/C catalysts. Furthermore, PtCo/NPC-Co showed excellent durability. The mass activity of PtCo/NPC-Co decreased by only 23% compared with that of Pt/C (49%) after 20,000 cycles. The interaction effect between NPC-Co and PtCo NPs enhanced the overall electrocatalytic performance. Additionally, the ORR mechanism is discussed in this study to advance our understanding of the electrocatalytic structure–activity relationship.

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Ultrahigh-permeance functionalized boron nitride membrane for nanoconfined heterogeneous catalysis

Cited by 30 publications

References 45 publications

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

Engineering Nanostructured Interfaces of Hexagonal Boron Nitride-Based Materials for Enhanced Catalysis

Angstrom-confined catalytic water purification within Co-TiOx laminar membrane nanochannels

Nitrogen-Doped Porous Carbon-Supported PtCo Nanoparticle Electrocatalyst for Oxygen Reduction Reaction Prepared by a Dual-Template Method

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