Palladium-based Catalytic Membrane Reactor for the continuous flow hydrodechlorination of chlorinated micropollutants

Nieto-Sandoval, Julia; Gomez‐Herrero, Esther; Pedro, Zahara M. de; Casas, J.A.

doi:10.1016/j.apcatb.2021.120235

Cited by 34 publications

(17 citation statements)

References 49 publications

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“…Generally, the exposure level of chlorinated organic pollutant (COP) contaminants is low (mg L –1 or even μg L –1 ) in the natural environment, and such a performance should therefore be far from satisfactory in practical applications. It has been well documented that the inferior performance of the above EHDC system in treating dilute 2,4-DCP originates from the short life of the H* radicals as well as the poor mass diffusion of 2,4-DCP in the normal batch reaction system, that is, a plate electrode drives the reaction in a stirred electrolyte solution . To address these issues, a membrane reactor for the continuous-flow EHDC reaction is customized (Figure a,b), where the catalyst is pasted into a thin membrane on a graphite plate (the current collector) and the contaminated water flows over the active membrane for the reaction.…”

Section: Resultsmentioning

confidence: 99%

“…It has been well documented that the inferior performance of the above EHDC system in treating dilute 2,4-DCP originates from the short life of the H* radicals 12 as well as the poor mass diffusion of 2,4-DCP in the normal batch reaction system, that is, a plate electrode drives the reaction in a stirred electrolyte solution. 8 To address these issues, a membrane reactor for the continuous-flow EHDC reaction is customized (Figure 6a,b), where the catalyst is pasted into a thin membrane on a graphite plate (the current collector) and the contaminated water flows over the active membrane for the reaction. Figure 6c shows that, within this system, 91.2% of the 2,4-DCP can be directly converted to phenol when fed 20.4 mg L −1 2,4-DCP, and the 2,4-DCP removal rate and F.E.…”

Section: Characterization Of Nimentioning

confidence: 99%

“…6,7 Current work primarily focuses on strategies to optimize the geometric and electronic states of Pd for intensified H* generation, which is dedicated to boosting the EHDC reaction and raising the atomic utilization efficiency of Pd. 8 Engineering Pd into nanowire/nanosheet structures, 9,10 alloying Pd with a promoting metal (Ag, In, and Cu), 11,12 constructing Pd-support interfaces (Pd−MnO 2 , 13 Pd−TiO 2 , 14 Pd−C 3 N 4 , 15 Pd−Ni 2 CoO 4 , 16 and Pd−TiN/TiC 17 ), decorating Pd with organic ligands, 18 sites 16,19−21 have all suggested to be efficient in affording high EHDC efficiencies. Despite these findings, little attention has been given to the H + supply chain.…”

Section: ■ Introductionmentioning

confidence: 99%

“…It has been well documented that the EHDC reaction is initiated by the reactive atomic hydrogen free radical (H*), which is generated in situ at the cathode surface via H + reduction on a specific catalyst, serving in hydrogenolysis of the C–Cl bond. , The noble metal palladium (Pd) is the priority catalyst for EHDC due to its relatively low energy barrier in H + /H* conversion, and its appropriate binding strength with H* that enables its evolution to H 2 to be slowed down. , Current work primarily focuses on strategies to optimize the geometric and electronic states of Pd for intensified H* generation, which is dedicated to boosting the EHDC reaction and raising the atomic utilization efficiency of Pd . Engineering Pd into nanowire/nanosheet structures, , alloying Pd with a promoting metal (Ag, In, and Cu), , constructing Pd-support interfaces (Pd–MnO 2 , Pd–TiO 2 , Pd–C 3 N 4 , Pd–Ni 2 CoO 4 , and Pd–TiN/TiC), decorating Pd with organic ligands, and creating atomically dispersed Pd sites ,− have all suggested to be efficient in affording high EHDC efficiencies.…”

Section: Introductionmentioning

confidence: 99%

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Defective Layered Double Hydroxide Nanosheet Boosts Electrocatalytic Hydrodechlorination Reaction on Supported Palladium Nanoparticles

Jiang

et al. 2022

ACS EST Water

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Electrocatalytic hydrodechlorination on Pd, utilizing the H + of H 2 O as hydrogen sources, represents a promising technology to detoxify the chlorinated organic pollutants (COPs) in water bodies. However, Pd alone affords limited activity due to its low efficacy in H 2 O disassociation and the poor mass diffusion of COPs that are commonly of low concentrations in the environment. Herein, we demonstrate that arming Pd with OH − vacancy-bearing NiAl-layered double hydroxide nanosheets (Pd/ Ni x Al 100−x -LDH-OH v ) can significantly improve its performance, benefiting from the enhanced H 2 O disassociation at OH v and the facilitated C−Cl cleavage on the supported Pd nanoparticles. Al 3+ is also indispensable because it promotes the formation and regeneration of OH v , but an overload will reduce the number of accessible OH v and weaken its function. Pd/Ni 67 Al 33 -LDH-OH v with the optimal Ni/Al ratio delivers a peak specific activity of 0.53 min −1 m −2 and mass activity of 6.54 min −1 g −1 Pd in treating 50.0 mg L −1 2,4-dichlorophenol (2,4-DCP, a probe COP) at −0.25 V versus RHE, outperforming most of the reported catalysts. To address the mass diffusion issue, Pd/Ni 67 Al 33 -LDH-OH v is integrated into a customized continuous-flow membrane cell. When fed a dilute wastewater (20.4 mg L −1 ), the system affords a 2,4-DCP removal rate of 3.75 g 2,4-DCP g catalyst −1 h −1 and faradaic current efficiency of 42.6%, which is 3.2 and 4.0 times that obtained in a traditional batch reaction system, respectively.

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Section: Resultsmentioning

confidence: 99%

Section: Characterization Of Nimentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Defective Layered Double Hydroxide Nanosheet Boosts Electrocatalytic Hydrodechlorination Reaction on Supported Palladium Nanoparticles

Jiang

et al. 2022

ACS EST Water

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“…The common catalysts used for HDC are supported noble metals, − for example, Pd, ,− Ru, and Rh, ,− while transition metals, such as Ni and Co, are effective for this reaction but require relatively critical reaction conditions. To achieve better performance, bimetallic alloy catalysts, for instance, PdAg, PtNi, NiFe, and PdNi, have also been studied, and their performances are usually dependent on the compositions of bimetallic alloys. , Among various catalysts, Pd has been recognized as efficient catalysts for HDC of various chlorophenols, which can be performed at atmospheric H 2 pressure and low temperatures.…”

Section: Introductionmentioning

confidence: 99%

Simultaneous Construction of Silica Nanotubes Loaded with Pd Nanoparticles for Catalytic Hydrodechlorination of Chlorophenols

Liu

et al. 2021

ACS Appl. Nano Mater.

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In this study, we for the first time use ditopic bis-terpyridine-containing metallopolymers as templates to synthesize metal nanoparticle-encapsulated nanoreactors. In the presence of the surfactant cetyltrimethylammonium bromide, the ditopic bis-terpyridines coordinate Pd 2+ ions to form linear metallopolymer bundles, which are further used as templates for silica deposition to give silicified Pd ion-containing tubular metallopolymers. The following calcination and subsequent reduction simultaneously result in Pd NP-encapsulated silica nanotubes (Pd-SNTs). Relative to the silica-supported Pd catalysts, the prepared Pd-SNTs demonstrate enhanced performance for hydrodechlorinations of various chlorophenols into phenolic compounds at 35 °C and atmospheric H 2 pressure and present high catalytic stability during five cycles of hydrodechlorination reactions.

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3D‐Continuous Nanoporous Covalent Framework Membrane Nanoreactors with Quantitatively Loaded Ultrafine Pd Nanocatalysts

Jeong,

Oh,

Park

2024

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The confinement effect of catalytic nanoreactors containing metal catalysts within nanometer‐sized volumes has attracted significant attention for their potential to enhance reaction rate and selectivity. Nevertheless, unregulated catalyst loading, aggregation, leaching, and limited reusability remain obstacles to achieving an efficient nanoreactor. A robust and durable catalytic membrane nanoreactor prepared by incorporating palladium nanocatalysts within a 3D‐continuous nanoporous covalent framework membrane is presented. The reduction of palladium precursor occurs on the pore surface within 3D nanochannels, producing ultrafine palladium nanoparticles (Pd NPs) with their number density adjustable by varying metal precursor concentrations. The precise catalyst loading enables controlling the catalytic activity of the reactor while preventing excess metal usage. The facile preparation of Pd NP‐loaded free‐standing membrane materials allows hydrodechlorination in both batch and continuous flow modes. In batch mode, the catalytic activity is proportional to the loaded Pd amount and membrane area, while the membrane retains its activity upon repeated use. In continuous mode, the conversion remains above 95% for over 100 h, with the reactant solution passing through a single 50 µm‐thick Pd‐loaded membrane. The efficient nanoporous film‐type catalytic nanoreactor may find applications in catalytic reactions for small chemical devices as well as in conventional chemistry and processes.

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Palladium-based Catalytic Membrane Reactor for the continuous flow hydrodechlorination of chlorinated micropollutants

Cited by 34 publications

References 49 publications

Defective Layered Double Hydroxide Nanosheet Boosts Electrocatalytic Hydrodechlorination Reaction on Supported Palladium Nanoparticles

Defective Layered Double Hydroxide Nanosheet Boosts Electrocatalytic Hydrodechlorination Reaction on Supported Palladium Nanoparticles

Simultaneous Construction of Silica Nanotubes Loaded with Pd Nanoparticles for Catalytic Hydrodechlorination of Chlorophenols

3D‐Continuous Nanoporous Covalent Framework Membrane Nanoreactors with Quantitatively Loaded Ultrafine Pd Nanocatalysts

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