Hydrogen spillover on N-doped carbon coating improves the hydrogenation performance of nickel catalysts

Author(s)

Arpini, Bruno Henrique ; Fiorio, Jhonatan Luiz ; da Costa, Joao Victor Ferreira ; Joswig, Jan-Ole ; Rossi, Liane Marcia

• Document type: Journal article
• Source: CATALYSIS SCIENCE & TECHNOLOGY; v. 14, n. 4, p. 9-pg., 2024-01-17.

Abstract

Improving the catalytic efficiency of earth-abundant metals, such as nickel, through surface design has the potential to replace noble-metal-based catalysts. Here, we report that coating nickel with nitrogen-doped carbon (Ni@NC) enhances its stability and activity for the semi-hydrogenation of phenylacetylene under mild conditions. Mechanistic studies with substituted phenylacetylenes revealed an electronic effect that suggests a contribution of the homolytic cleavage of H2 followed by hydrogen spillover to the N-doped carbon coating. As a result, the hydrogenation reaction occurs at temperatures as low as 25 degrees C, while the benchmark RANEY (R) nickel is inactive. These results are supported by a combination of experimental results and theoretical insights. Moreover, this efficient hydrogenation catalyst is resistant to carbon monoxide poisoning and remains active even at low temperatures. Ni@N-doped carbon exhibits superior hydrogenation activity than RANEY (R) nickel. The high activity was attributed to hydrogen spillover from Ni to N-doped carbon, which also enhances CO poisoning resistance. (AU)

• FAPESP's process: 20/15230-5 - Research Centre for Greenhouse Gas Innovation - RCG2I
• Grantee: Julio Romano Meneghini
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 18/26253-6 - COOPERATIVE CATALYSIS: AN ALTERNATIVE FOR THE DEVELOPMENT OF GOLD AND EARTH-ABUNDANT TRANSITION METAL CATALYSTS
• Grantee: Liane Marcia Rossi
• Support Opportunities: Regular Research Grants
• FAPESP's process: 17/24348-7 - Development of hybrid catalysts for conversion of CO2 into chemicals and fuels
• Grantee: Bruno Henrique Arpini
• Support Opportunities: Scholarships in Brazil - Doctorate
• FAPESP's process: 14/50279-4 - Brasil Research Centre for Gas Innovation
• Grantee: Julio Romano Meneghini
• Support Opportunities: Research Grants - Research Centers in Engineering Program
• FAPESP's process: 21/00675-4 - Tying up materials for electrochemical energy storage and catalysis
• Grantee: Roberto Manuel Torresi
• Support Opportunities: Research Projects - Thematic Grants