Porosity Engineering Within Ni─N─C Hollow Spheres for Ampere‐Level CO <sub>2</sub> Reduction Electrocatalysis
Abstract
ABSTRACT CO 2 electroreduction typically requires large overpotentials to sustain high reaction rates, which at current densities approaching 1 A cm −2 inevitably intensify competition from the hydrogen evolution reaction (HER), making it difficult to simultaneously sustain high product selectivity (>95%). In this study, hollow Ni─NC (H‐Ni‐NC) was synthesized using nanoscale silica sphere templates and atomic Zn as a sacrificial pore‐former within the carbon shell. The optimized H‐Ni‐NC achieves a current density of −1.0 A cm −2 with over 95% CO Faradaic efficiency in a flow cell. The high performance was attributed to the hollow sphere architecture enriched with gas‐permeable through‐pores. Notably, the Zn dosage selectively modulates the shell through‐porosity, without altering hollow sphere macrostructure or the active‐site structure, thereby enabling a systematic investigation of porosity effects. Finite‐element simulations provide a qualitative framework suggesting a trade‐off between reactant transport and active surface area with increasing porosity in hollow spherical catalysts. This work underscores that engineering of the nanoscale mass‐transport environment surrounding active sites plays a critical role in designing high‐efficiency electrocatalysts.
Article Details
Authors (14)
Jiage Yu
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
Wei Liu
Lu Bai
Beijing Key Laboratory of Solid-State Battery and Energy Storage Process, Key Laboratory of Green Process and Engineering, State Key Laboratory of Mesoscience and Process Engineering
Benqiang Tian
State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing P. R. China
Qingyi Zhu
Department of Chemistry
Qianxi Yang
State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology Beijing P. R. China
Linlin Zhou
Haoyang Wu
Institute for Advanced Materials and Technology
Yuan Wang
Boyuan Li
Frontiers Science Center for New Organic Matter, State Key Laboratory of Advanced Chemical Power Sources, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Academy of Advanced Inter Disciplinary Studies, College of Chemistry
Xiangrong Jin
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
Yun Kuang
Ocean Hydrogen Energy R&D Center
Jiazhan Li
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
Xiaoming Sun