Electrocatalytic Hydrogenation of Phenol over Platinum and Rhodium: Unexpected Temperature Effects Resolved

Nirala Singh; Yang Song; Oliver Y. Gutiérrez; Donald M. Camaioni; Charles T. Campbell; Johannes A. Lercher

doi:10.1021/acscatal.6b02296

Electrocatalytic Hydrogenation of Phenol over Platinum and Rhodium: Unexpected Temperature Effects Resolved

Nirala Singh, Yang Song, Oliver Y. Gutiérrez, Donald M. Camaioni, Charles T. Campbell, Johannes A. Lercher

Chair of Chemical Technology II

Research output: Contribution to journal › Article › peer-review

87 Scopus citations

Abstract

Both electrocatalytic hydrogenation (ECH) and thermal catalytic hydrogenation (TCH) of phenol by Pt and Rh show a rollover in rate with increasing temperature without changing the principal reaction pathways. The negative effect of temperature for aqueous-phase phenol TCH and ECH on Pt and Rh is deduced to be from dehydrogenated phenol adsorbates, which block active sites. ECH and TCH rates increase similarly with increasing hydrogen chemical potential whether induced by applied potential or H₂ pressure, both via increasing H coverage, and indirectly by removing site blockers, a strong effect at high temperature. This enables unprecedented phenol TCH rates at 60-100°C. (Graph Presented).

Original language	English
Pages (from-to)	7466-7470
Number of pages	5
Journal	ACS Catalysis
Volume	6
Issue number	11
DOIs	https://doi.org/10.1021/acscatal.6b02296
State	Published - 4 Nov 2016

Keywords

electrocatalysis
hydrogenation
phenol
platinum
poisoning
rhodium

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title = "Electrocatalytic Hydrogenation of Phenol over Platinum and Rhodium: Unexpected Temperature Effects Resolved",

abstract = "Both electrocatalytic hydrogenation (ECH) and thermal catalytic hydrogenation (TCH) of phenol by Pt and Rh show a rollover in rate with increasing temperature without changing the principal reaction pathways. The negative effect of temperature for aqueous-phase phenol TCH and ECH on Pt and Rh is deduced to be from dehydrogenated phenol adsorbates, which block active sites. ECH and TCH rates increase similarly with increasing hydrogen chemical potential whether induced by applied potential or H2 pressure, both via increasing H coverage, and indirectly by removing site blockers, a strong effect at high temperature. This enables unprecedented phenol TCH rates at 60-100°C. (Graph Presented).",

keywords = "electrocatalysis, hydrogenation, phenol, platinum, poisoning, rhodium",

author = "Nirala Singh and Yang Song and Guti{\'e}rrez, {Oliver Y.} and Camaioni, {Donald M.} and Campbell, {Charles T.} and Lercher, {Johannes A.}",

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doi = "10.1021/acscatal.6b02296",

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TY - JOUR

T1 - Electrocatalytic Hydrogenation of Phenol over Platinum and Rhodium

T2 - Unexpected Temperature Effects Resolved

AU - Singh, Nirala

AU - Song, Yang

AU - Gutiérrez, Oliver Y.

AU - Camaioni, Donald M.

AU - Campbell, Charles T.

AU - Lercher, Johannes A.

PY - 2016/11/4

Y1 - 2016/11/4

N2 - Both electrocatalytic hydrogenation (ECH) and thermal catalytic hydrogenation (TCH) of phenol by Pt and Rh show a rollover in rate with increasing temperature without changing the principal reaction pathways. The negative effect of temperature for aqueous-phase phenol TCH and ECH on Pt and Rh is deduced to be from dehydrogenated phenol adsorbates, which block active sites. ECH and TCH rates increase similarly with increasing hydrogen chemical potential whether induced by applied potential or H2 pressure, both via increasing H coverage, and indirectly by removing site blockers, a strong effect at high temperature. This enables unprecedented phenol TCH rates at 60-100°C. (Graph Presented).

AB - Both electrocatalytic hydrogenation (ECH) and thermal catalytic hydrogenation (TCH) of phenol by Pt and Rh show a rollover in rate with increasing temperature without changing the principal reaction pathways. The negative effect of temperature for aqueous-phase phenol TCH and ECH on Pt and Rh is deduced to be from dehydrogenated phenol adsorbates, which block active sites. ECH and TCH rates increase similarly with increasing hydrogen chemical potential whether induced by applied potential or H2 pressure, both via increasing H coverage, and indirectly by removing site blockers, a strong effect at high temperature. This enables unprecedented phenol TCH rates at 60-100°C. (Graph Presented).

KW - electrocatalysis

KW - hydrogenation

KW - phenol

KW - platinum

KW - poisoning

KW - rhodium

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DO - 10.1021/acscatal.6b02296

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JO - ACS Catalysis

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ER -

Electrocatalytic Hydrogenation of Phenol over Platinum and Rhodium: Unexpected Temperature Effects Resolved

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