PMID- 37844151
OWN - NLM
STAT- MEDLINE
DCOM- 20231101
LR  - 20231106
IS  - 1520-5851 (Electronic)
IS  - 0013-936X (Linking)
VI  - 57
IP  - 43
DP  - 2023 Oct 31
TI  - Enhanced Hydrosaturation Selectivity and Electron Transfer for Electrocatalytic 
      Chlorophenols Hydrogenation on Ru Sites.
PG  - 16695-16706
LID - 10.1021/acs.est.3c06669 [doi]
AB  - Electrocatalytic hydrogenation is acknowledged as a promising strategy for 
      chlorophenol dechlorination. However, the widely used Pd catalysts exhibit 
      drawbacks, such as high costs and low selectivity for phenol hydrosaturation. 
      Herein, we demonstrate the potential and mechanism of Ru in serving as a Pd 
      substitute using 2,4,6-trichlorophenol (TCP) as a model pollutant. Up to 99.8% 
      TCP removal efficiency and 99% selectivity to cyclohexanol, a value-added 
      compound with an extremely low toxicity, were achieved on the Ru electrode. In 
      contrast, only 66% of TCP was removed on the Pd electrode, with almost no 
      hydrosaturation selectivity. The superiority of Ru over Pd was especially 
      noteworthy in alkaline conditions or the presence of interfering species such as 
      S(2-). The theoretical simulation demonstrates that Ru possesses a 
      hydrodechlorination energy barrier of 0.72 eV, which is comparable to that on Pd. 
      Meanwhile, hydrosaturation requires an activation energy of 0.69 eV on Ru, which 
      is much lower than that on Pd (0.92 eV). The main reaction mechanism on Ru is 
      direct electron transfer, which is distinct from that on Pd (indirect pathway via 
      atomic hydrogen, H*). This work thereby provides new insights into designing 
      cost-effective electrocatalysts for halogenated phenol detoxification and 
      resource recovery.
FAU - Gu, Zhenao
AU  - Gu Z
AUID- ORCID: 0000-0002-8853-4204
AD  - State Key Laboratory of Environmental Aquatic Chemistry, Research Center for 
      Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
AD  - University of Chinese Academy of Sciences, Beijing 100049, China.
AD  - National Engineering Research Center of Industrial Wastewater Detoxication and 
      Resource Recovery, Beijing 100085, China.
FAU - Ni, Nan
AU  - Ni N
AD  - State Key Laboratory of Environmental Aquatic Chemistry, Research Center for 
      Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
AD  - School of Environmental and Municipal Engineering, Xi'an University of 
      Architecture and Technology, Xi'an 710055, China.
FAU - He, Guangzhi
AU  - He G
AUID- ORCID: 0000-0003-1770-3522
AD  - State Key Joint Laboratory of Environment Simulation and Pollution Control, 
      Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, 
      Beijing 100085, China.
AD  - University of Chinese Academy of Sciences, Beijing 100049, China.
FAU - Shan, Yulong
AU  - Shan Y
AUID- ORCID: 0000-0002-5031-8522
AD  - State Key Joint Laboratory of Environment Simulation and Pollution Control, 
      Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, 
      Beijing 100085, China.
FAU - Wu, Kun
AU  - Wu K
AD  - School of Environmental and Municipal Engineering, Xi'an University of 
      Architecture and Technology, Xi'an 710055, China.
FAU - Hu, Chengzhi
AU  - Hu C
AUID- ORCID: 0000-0001-9898-835X
AD  - State Key Laboratory of Environmental Aquatic Chemistry, Research Center for 
      Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
AD  - University of Chinese Academy of Sciences, Beijing 100049, China.
AD  - National Engineering Research Center of Industrial Wastewater Detoxication and 
      Resource Recovery, Beijing 100085, China.
FAU - Qu, Jiuhui
AU  - Qu J
AUID- ORCID: 0000-0001-9177-093X
AD  - State Key Laboratory of Environmental Aquatic Chemistry, Research Center for 
      Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.
AD  - University of Chinese Academy of Sciences, Beijing 100049, China.
LA  - eng
PT  - Journal Article
PT  - Research Support, Non-U.S. Gov't
DEP - 20231016
PL  - United States
TA  - Environ Sci Technol
JT  - Environmental science & technology
JID - 0213155
RN  - 0 (Chlorophenols)
RN  - 339NCG44TV (Phenol)
SB  - IM
MH  - *Chlorophenols
MH  - Hydrogenation
MH  - Electrons
MH  - Phenol
MH  - Electron Transport
OTO - NOTNLM
OT  - atomic hydrogen
OT  - chlorophenols
OT  - detoxification
OT  - direct electron transfer
OT  - hydrodechlorination
OT  - hydrosaturation
OT  - resource recovery
EDAT- 2023/10/16 18:42
MHDA- 2023/11/01 12:43
CRDT- 2023/10/16 14:12
PHST- 2023/11/01 12:43 [medline]
PHST- 2023/10/16 18:42 [pubmed]
PHST- 2023/10/16 14:12 [entrez]
AID - 10.1021/acs.est.3c06669 [doi]
PST - ppublish
SO  - Environ Sci Technol. 2023 Oct 31;57(43):16695-16706. doi: 
      10.1021/acs.est.3c06669. Epub 2023 Oct 16.