Ni Single-Atoms Supported on N-Doped Carbon Prepared by Cation Exchange: Ultrafast Catalyst For The Reduction of Nitroarene Compounds Under Ambient Conditions

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Batista, Walker Vinicius Ferreira do Carmo ; de Oliveira, Wanessa Lima ; de Oliveira, Eduarda Ferreira ; Cruz, Tais Santos ; Ferrari, Jefferson Luis ; Archanjo, Braulio Soares ; Grigoletto, Sabrina ; Ferreira, Dalva Ester da Costa ; Pereira, Fabiano Vargas ; Diab, Gabriel Ali Atta ; Mastelaro, Valmor Roberto ; Teixeira, Ivo Freitas ; de Mesquita, Joao Paulo

• Document type: Journal article
• Source: CHEMCATCHEM; v. 16, n. 18, p. 13-pg., 2024-07-16.

Abstract

We present a highly efficient single-atom catalyst (SACs) tailored for nitroarene reduction using NaBH4 under ambient conditions. Employing an unique approach, we harnessed NaCl under high temperature to create host materials enriched with negatively charged nitrogenous and oxygenated functional groups, capable of anchoring and stabilizing Ni ions within the aromatic structure. The nickel single sites were prepared by a straightforward cation exchange method. STEM-HAADF imaging confirmed the presence of nickel single-atoms, while XPS, FTIR, and Raman spectra validated nickel coordination within the catalyst. Remarkably, the CN-Ni catalyst exhibited exceptional catalytic performance under ambient conditions, achieving a high catalytic activity with NaBH4 (TOF 2246 +/- ${\pm }$ 452 h-1 and 107 +/- ${\pm }$ 47 mmol g-1 min-1). It also demonstrated remarkable conversion exceeding 90 % and outstanding selectivity. Equally impressive was its ability to maintain full catalytic activity over multiple reaction cycles, highlighting its robustness. This work is a significant leap in SACs design, offering a versatile and highly effective preparation method for SACs based on N-doped carbon with far-reaching implications in industrial reduction reactions. A new strategy to stabilize nickel single-atoms in N-doped carbon synthesized employing NaCl to generate hosts with negatively charged N-doped carbon. This synthesis method led to highly efficient nickel species for the reduction of nitroarenes (TOF 2246 h-1). image (AU)

• FAPESP's process: 21/14006-7 - PHI/PTI-single-atoms controlled synthesis and energy applications
• Grantee: Gabriel Ali Atta Diab
• Support Opportunities: Scholarships in Brazil - Doctorate (Direct)
• FAPESP's process: 21/12394-0 - Sustainable synthetic methods employing catalysis, benign solvents, safer reagents, and bio-renewable feedstock
• Grantee: Arlene Gonçalves Corrêa
• Support Opportunities: Research Projects - Thematic Grants
• FAPESP's process: 20/14741-6 - Graphitic carbon nitrides as platforms for single-atom photocatalysis: moving towards design principles for improved performance
• Grantee: Ivo Freitas Teixeira
• Support Opportunities: Research Grants - Young Investigators Grants
• FAPESP's process: 21/13271-9 - Single atoms coordinated on graphitic carbon nitrides to photocatalytic conversion of methane
• Grantee: Marcos Augusto Ribeiro da Silva
• Support Opportunities: Scholarships in Brazil - Doctorate