Kinetics and mechanisms of electrocatalytic hydrodechlorination of diclofenac on Pd-Ni/PPy-rGO/Ni electrodes

Li, Junjing; Wang, Huan; Qi, Ziyan; Ma, Chao; Zhang, Zhaohui; Zhao, Bin; Wang, Liang; Zhang, Hongwei; Chong, Yutong; Chen, Xiang; Cheng, Xiuwen; Dionysiou, Dionysios D.

doi:10.1016/j.apcatb.2020.118696

Cited by 64 publications

(23 citation statements)

References 57 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In fact, this pair was visible only after applying more negative potentials and upon the emergence of the H* peak. This highlights the role of H* as an active reactant for hydrodechlorination, which has been reported for Pd nanoparticles. , Overall, Figure a,b demonstrates that both pathways, direct cathodic reduction and indirect hydrogenation involving H*, are involved for 4-CP hydrodechlorination on Pd 1 /rGO.…”

Section: Results and Discussionsupporting

confidence: 67%

“…This highlights the role of H* as an active reactant for hydrodechlorination, which has been reported for Pd nanoparticles. 61,62 Overall, Figure 4a,b demonstrates that both pathways, direct cathodic reduction and indirect hydrogenation involving H*, are involved for 4-CP hydrodechlorination on Pd 1 /rGO. Pd 1 /rGO was further compared to Pd nano /rGO by performing CV at the same total catalyst mass loading (Figure 4c).…”

Section: ■ Experimentalmentioning

confidence: 93%

See 1 more Smart Citation

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Huang

Kim

Rigby

et al. 2021

Environ. Sci. Technol.

View full text Add to dashboard Cite

In this study, we loaded Pd catalysts onto a reduced graphene oxide (rGO) support in an atomically dispersed fashion [i.e., Pd single-atom catalysts (SACs) on rGO or Pd 1 /rGO] via a facile and scalable synthesis based on anchor-site and photoreduction techniques. The as-synthesized Pd 1 /rGO significantly outperformed the Pd nanoparticle (Pd nano ) counterparts in the electrocatalytic hydrodechlorination of chlorinated phenols. Downsizing Pd nano to Pd 1 leads to a substantially higher Pd atomic efficiency (14 times that of Pd nano ), remarkably reducing the cost for practical applications. The unique single-atom architecture of Pd 1 additionally affects the desorption energy of the intermediate, suppressing the catalyst poisoning by Cl − , which is a prevalent challenge with Pd nano . Characterization and experimental results demonstrate that the superior performance of Pd 1 /rGO originates from (1) enhanced interfacial electron transfer through Pd−O bonds due to the electronic metal−support interaction and (2) increased atomic H (H*) utilization efficiency by inhibiting H 2 evolution on Pd 1 . This work presents an important example of how the unique geometric and electronic structure of SACs can tune their catalytic performance toward beneficial use in environmental remediation applications.

show abstract

Section: Results and Discussionsupporting

confidence: 67%

Section: ■ Experimentalmentioning

confidence: 93%

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Huang

Kim

Rigby

et al. 2021

Environ. Sci. Technol.

View full text Add to dashboard Cite

show abstract

“…Further addition of the active H ads * atoms breaks the Pd–C bonds and forms H–C bonds, which leads to desorption of the products from the PdNP surface to the aqueous phase (steps ⑤ and ⑥ in Figure ) …”

Section: Resultsmentioning

confidence: 99%

Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H₂-Transfer Membranes

Luo

Zhou

et al. 2020

Environ. Sci. Technol.

View full text Add to dashboard Cite

TCA) and trichloroethene (TCE) are common recalcitrant contaminants that coexist in groundwater. H 2 -induced reduction over precious-metal catalysts has proven advantageous, but its application to long-term continuous treatment has been limited due to poor H 2 -transfer efficiency and catalyst loss. Furthermore, catalytic reductions of aqueous 1,1,1-TCA alone or concomitant with TCE catalytic co-reductions are unstudied. Here, we investigated 1,1,1-TCA and TCE co-reduction using palladium nanoparticle (PdNP) catalysts spontaneously deposited on H 2 -transfer membranes that allow efficient H 2 supply on demand in a bubble-free form. The catalytic activities for 1,1,1-TCA and TCE reductions reached 9.9 and 11 L/g-Pd/min, values significantly greater than that reported for other immobilized-PdNP systems. During 90 day continuous operation, removals were up to 95% for 1,1,1-TCA and 99% for TCE. The highest steady-state removal fluxes were 1.5 g/ m 2 /day for 1,1,1-TCA and 1.7 g/m 2 /day for TCE. The major product was nontoxic ethane (94% selectivity). Only 4% of the originally deposited PdNPs were lost over 90 days of continuous operation. Documenting long-term continuous Pd-catalyzed dechlorination at high surface loading with minimal loss of the catalyst mass or activity, this work expands understanding of and provides a foundation for sustainable catalytic removal of co-existing chlorinated solvents.

show abstract

“…•and •OH, resulting in a decreased oxidation rate of organic compounds (Fabianśka et al 2015), as well as DCF. Li et al (2020c) also found that HCO 3 À showed inhibitory effect of electrocatalytic hydrodechlorination of diclofenac on Pd-Ni/PPy-rGO/Ni electrodes. When 5 mmol L À1 of HCO 3 À were added, the kinetics and removal rate were lower than with 0.1 mmol L À1 of HCO 3 À added but higher than with 1 mmol L À1 of HCO 3 À .…”

Section: Effects Of Electrode Spacing On Dcf Degradationmentioning

confidence: 84%

“…Adsorption and advanced oxidation process such as photodegaradation are commonly known methods for the removal of pharmaceutical drugs (Ali et al 2016;Sharma et al 2018;Balasubramani et al 2020;Dhiman et al 2021). Ultrasonic, ozonation, the Fenton process, photocatalysis, chlorine oxidation and electrolysis have been studied to examine and compare the removal effect on DCF (Huber et al 2003;Brillas et al 2010;Nie et al 2014;Wang et al 2014;Wang et al 2015a;Kumar et al 2020;Li et al 2020aLi et al , 2020b.…”

Section: Graphical Abstract Introductionmentioning

confidence: 99%

Electrochemical degradation of DCF by boron-doped diamond anode: degradation mechanism, pathways and influencing factors

Qiu

Fan

et al. 2021

Water Science and Technology

View full text Add to dashboard Cite

Nonsteroidal anti-inflammatory drugs (NAIDS) have been widely detected in wastewater and surface water, which indicates the removal of NAIDS by wastewater treatment plants was not efficiency. Electrochemical advanced oxidation technology is considered to be an effective process. This study presents an investigation of the kinetics, mechanism and influencing factors of Diclofenac (DCF) degradation by an electrochemical process with the boron doped diamond anodes. Relative operating parameters and water quality parameters are examined. It appears that the degradation follows the pseudo-first-order degradation kinetics. DCF degradation was accelerated with the increase of pH from 6 to 10. The degradation was promoted by the addition of electrolyte concentrations and current density. HA and HCO3− significantly inhibited the degradation, whereas Cl− accelerated it. According to the inhibition tests, hydroxyl radicals (•OH) and sulfate radicals (SO4•–) contributed 76.5% and 6.5%, respectively, to the degradation. Sodium sulphate remains a more effective electrolyte, compared to sodium nitrate and sodium phosphate, suggesting the quenching effect of nitrate and phosphate on •OH. Major DCF transformation products were identified. According to the degradation products detected by liquid chromatography-mass spectrometry, hydroxylation and decarboxylation are the main pathways to DCF degradation; meanwhile, dechlorination, chlorination and nitro substitution are also included.

show abstract

Kinetics and mechanisms of electrocatalytic hydrodechlorination of diclofenac on Pd-Ni/PPy-rGO/Ni electrodes

Cited by 64 publications

References 57 publications

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H₂-Transfer Membranes

Electrochemical degradation of DCF by boron-doped diamond anode: degradation mechanism, pathways and influencing factors

Contact Info

Product

Resources

About

Kinetics and mechanisms of electrocatalytic hydrodechlorination of diclofenac on Pd-Ni/PPy-rGO/Ni electrodes

Cited by 64 publications

References 57 publications

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Elucidating the Role of Single-Atom Pd for Electrocatalytic Hydrodechlorination

Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H2-Transfer Membranes

Electrochemical degradation of DCF by boron-doped diamond anode: degradation mechanism, pathways and influencing factors

Contact Info

Product

Resources

About

Long-Term Continuous Co-reduction of 1,1,1-Trichloroethane and Trichloroethene over Palladium Nanoparticles Spontaneously Deposited on H₂-Transfer Membranes