PMID- 33438993
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20210128
IS  - 1944-8252 (Electronic)
IS  - 1944-8244 (Linking)
VI  - 13
IP  - 3
DP  - 2021 Jan 27
TI  - Surface Ligand Environment Boosts the Electrocatalytic Hydrodechlorination 
      Reaction on Palladium Nanoparticles.
PG  - 4072-4083
LID - 10.1021/acsami.0c20994 [doi]
AB  - We present an enhanced catalytic efficiency of palladium (Pd) nanoparticles (NPs) 
      for the electrocatalytic hydrodechlorination (EHDC) reaction by incorporating the 
      tetraethylammonium chloride (TEAC) ligand into the surface of NPs. Both 
      experimental and theoretical analyses reveal that the surface-adsorbed TEAC is 
      converted to molecular amine (primarily triethylamine) under reductive 
      potentials, forming a strong ligand-Pd interaction that is beneficial to the EHDC 
      kinetics. Using the EHDC of 2,4-dichlorophenol (2,4-DCP), a dominant persistent 
      pollutant identified by the U.S. Environmental Protection Agency, as an example, 
      the Pd/amine composite delivers a mass activity of 2.32 min(-1) g(Pd)(-1) and a 
      specific activity of 0.16 min(-1) cm(-2) at -0.75 V versus Ag/AgCl, outperforming 
      Pd and most of the previously reported catalysts. The mechanistic study reveals 
      that the amine ligand offers three functions: the H(+)-pumping effect, the 
      electronic effect, and the steric effect, providing a favorable environment for 
      the generation of reactive hydrogen radicals (H*) for hydrogenolysis of the C-Cl 
      bond. It also weakens the adsorption strength of EHDC products, alleviating their 
      poisoning on Pd. Investigation into the intermediate products of EHDC on Pd/amine 
      and the biological safety of the 2,4-DCP-contaminated water after EHDC treatment 
      demonstrates that EHDC on Pd/amine is environmentally benign for halogenated 
      organic pollutant abatement. This work suggests that the tuning of NP catalysis 
      using facile ligand post-treatment may lead to new strategies to improve EHDC for 
      environmental remediation applications.
FAU - Jiang, Guangming
AU  - Jiang G
AUID- ORCID: 0000-0002-7375-0107
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Shi, Xuelin
AU  - Shi X
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Cui, Meiyang
AU  - Cui M
AD  - Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, 
      United States.
FAU - Wang, Weilu
AU  - Wang W
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Wang, Peng
AU  - Wang P
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Johnson, Grayson
AU  - Johnson G
AUID- ORCID: 0000-0001-5229-1135
AD  - Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, 
      United States.
FAU - Nie, Yudong
AU  - Nie Y
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Lv, Xiaoshu
AU  - Lv X
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Zhang, Xianming
AU  - Zhang X
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Dong, Fan
AU  - Dong F
AUID- ORCID: 0000-0003-2890-9964
AD  - Engineering Research Center for Waste Oil Recovery Technology and Equipment, 
      Ministry of Education, Chongqing Technology and Business University, Chongqing 
      400067,China.
FAU - Zhang, Sen
AU  - Zhang S
AUID- ORCID: 0000-0002-1716-3741
AD  - Department of Chemistry, University of Virginia, Charlottesville, Virginia 22904, 
      United States.
LA  - eng
PT  - Journal Article
DEP - 20210113
PL  - United States
TA  - ACS Appl Mater Interfaces
JT  - ACS applied materials & interfaces
JID - 101504991
SB  - IM
OTO - NOTNLM
OT  - electrocatalysis
OT  - hydrodechlorination
OT  - ligand modification
OT  - palladium
OT  - reactive hydrogen species
EDAT- 2021/01/14 06:00
MHDA- 2021/01/14 06:01
CRDT- 2021/01/13 12:10
PHST- 2021/01/14 06:00 [pubmed]
PHST- 2021/01/14 06:01 [medline]
PHST- 2021/01/13 12:10 [entrez]
AID - 10.1021/acsami.0c20994 [doi]
PST - ppublish
SO  - ACS Appl Mater Interfaces. 2021 Jan 27;13(3):4072-4083. doi: 
      10.1021/acsami.0c20994. Epub 2021 Jan 13.