Abstract
Materials innovation plays an essential role to address the increasing demands of gaseous chlorine from anodic chlorine evolution reaction (CER) in chlor-alkali electrolysis. In this study, two-dimensional (2D) semiconducting group-VA monolayers were theoretically screened for the electrochemical CER by means of the density functional theory (DFT) method. Our results reveal the monolayered β-arsenene has the ultralow thermodynamic overpotential of 0.068 V for CER, which is close to that of the commercial Ru/Ir-based dimensionally stable anode (DSA) of 0.08 V @ 10 mA cm−2 and 0.13 V from experiments and theory, respectively. The change of CER pathways via Cl* intermediate on 2D β-arsenene also efficiently suppresses the parasitical oxygen gas production because of a high theoretical oxygen evolution reaction (OER) overpotential of 1.95 V. Our findings may therefore expand the scope of the electrocatalysts design for CER by using emerging 2D materials.
Highlights
The chlor-alkali process as the primary means for chlorine (Cl2) manufacture is one of the largest industrial electrochemical technologies [1,2]
Electrocatalysis is the heart of the cost-intensive chlor-alkali industry since it has the demonstrated capacity for a series of energy-related applications including chlorine evolution reaction (CER), oxygen reduc-tion reaction (ORR), and hydrogen evolution reaction (HER) [3–6]
Our calculated results reveal that β-arsenene monolayer exhibits high activity and selectivity of gaseous Cl2 generation by virtue of the expected Cl* precursor, with the thermodynamic overpotential of 0.068 V and 1.95 V for the CER and oxygen evolution reaction (OER), respectively
Summary
The chlor-alkali process as the primary means for chlorine (Cl2) manufacture is one of the largest industrial electrochemical technologies [1,2]. The DSA catalysts have a high oxygen evolution reaction (OER) activity [1,12–16]. To solve the encountered selectivity issue, one of the most promising strategies is the acidification of electrolyte solutions, as the OER perfor-mance of most electrode materials can be suppressed in an acidic media, while the reversible electrode potential of CER is pH-independent [9,19]. To this end, the screening of novel high-performance CER with high reactivity and selectivity in acidic solution be-comes imperative. Our DFT results predict that the 2D β-arsenene monolayer is a promising candidate for CER with the ultralow thermodynamic overpotential of 0.068 V and high selectivity in terms of OER
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