PMID- 28541678 OWN - NLM STAT- MEDLINE DCOM- 20180112 LR - 20181202 IS - 1520-5851 (Electronic) IS - 0013-936X (Linking) VI - 51 IP - 13 DP - 2017 Jul 5 TI - Identification of Active Hydrogen Species on Palladium Nanoparticles for an Enhanced Electrocatalytic Hydrodechlorination of 2,4-Dichlorophenol in Water. PG - 7599-7605 LID - 10.1021/acs.est.7b01128 [doi] AB - Clarifying hydrogen evolution and identifying the active hydrogen species are crucial to the understanding of the electrocatalytic hydrodechlorination (EHDC) mechanism. Here, monodisperse palladium nanoparticles (Pd NPs) are used as a model catalyst to demonstrate the potential-dependent evolutions of three hydrogen species, including adsorbed atomic hydrogen (H*(ads)), absorbed atomic hydrogen (H*(abs)), and molecular hydrogen (H(2)) on Pd NPs, and then their effect on EHDC of 2,4-dichlorophenol (2,4-DCP). Our results show that H*(ads), H*(abs), and H(2) all emerge at -0.65 V (vs Ag/AgCl) and have increased amounts at more negative potentials, except for H*(ads) that exhibits a reversed trend with the potential varying from -0.85 to -0.95 V. Overall, the concentrations of these three species evolve in an order of H*(abs) < H*(ads) < H(2) in the potential range of -0.65 to -0.85 V, H*(ads) < H*(abs) < H(2) in -0.85 to -1.00 V, and H*(ads) < H(2) < H*(abs) in -1.00 to -1.10 V. By correlating the evolution of each hydrogen species with 2,4-DCP EHDC kinetics and efficiency, we find that H*(ads) is the active species, H*(abs) is inert, while H(2) bubbles are detrimental to the EHDC reaction. Accordingly, for an efficient EHDC reaction, a moderate potential is desired to yield sufficient H*(ads) and limit H(2) negative effect. Our work presents a systematic investigation on the reaction mechanism of EHDC on Pd catalysts, which should advance the application of EHDC technology in practical environmental remediation. 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 - Lan, Mengna AU - Lan M AD - Engineering Research Center for Waste Oil Recovery Technology and Equipment, Ministry of Education, Chongqing Technology and Business University , Chongqing 400067, China. FAU - Zhang, Zhiyong AU - Zhang Z AD - Department of Chemistry, University of Virginia , Charlottesville, Virginia 22904, United States. 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 - Lou, Zimo AU - Lou Z AD - Department of Environmental Engineering, Zhejiang University , Hangzhou 310058, China. FAU - Xu, Xinhua AU - Xu X AD - Department of Environmental Engineering, Zhejiang University , Hangzhou 310058, China. FAU - Dong, Fan AU - Dong F 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 AD - Department of Chemistry, University of Virginia , Charlottesville, Virginia 22904, United States. LA - eng PT - Journal Article DEP - 20170613 PL - United States TA - Environ Sci Technol JT - Environmental science & technology JID - 0213155 RN - 0 (Chlorophenols) RN - 059QF0KO0R (Water) RN - 5TWQ1V240M (Palladium) RN - 7YNJ3PO35Z (Hydrogen) RN - R669TG1950 (2,4-dichlorophenol) SB - IM MH - Catalysis MH - Chlorophenols/*chemistry MH - Hydrogen MH - Nanoparticles/*chemistry MH - Palladium MH - Water EDAT- 2017/05/26 06:00 MHDA- 2018/01/13 06:00 CRDT- 2017/05/26 06:00 PHST- 2017/05/26 06:00 [pubmed] PHST- 2018/01/13 06:00 [medline] PHST- 2017/05/26 06:00 [entrez] AID - 10.1021/acs.est.7b01128 [doi] PST - ppublish SO - Environ Sci Technol. 2017 Jul 5;51(13):7599-7605. doi: 10.1021/acs.est.7b01128. Epub 2017 Jun 13.