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Enhanced nitrite electroreduction to ammonia via interfacial dual-site adsorption

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The nitrite(NO2-)to ammonia(NH3)electroreduction reaction(NO2-RR)would be impeded by sluggish proton-coupled electron transfer kinetics and competitive hydrogen evolution reaction(HER).A key to improving the NH3 selectivity is to facilitate adsorption and activation of NO2-,which is generally unde-sirable in unitary species.In this work,an efficient NO2-RR catalyst is constructed by cooperating Pd with In2O3,in which NO2 could adsorb on interfacial dual-site through"Pd-N-O-In"linkage,leading to strengthened NO2-adsorption and easier N=O bond cleavage than that on unitary Pd or In2O3.Moreover,the Pd/In2O3 composite exhibits moderate H* adsorption,which may facilitate protonation kinetics while inhibiting competitive HER.As a result,it exhibits a fairly high NH3 yield rate of 622.76 mmol h-1 gca1 with a Faradaic efficiency(FE)of 95.72％,good selectivity of 91.96％,and cycling sta-bility towards the NO2-RR,surpassing unitary In2O3 and Pd/C electrocatalysts.Besides,computed results indicate that NH3 production on Pd/In2O3 follows the deoxidation to hydrogenation pathway.This work highlights the significance of H* and NO2 adsorption modulation and N=O activation in NO2-RR electro-chemistry by creating synergy between a mediocre catalyst with an appropriate cooperator.

Dual-site adsorptionNitrite electroreductionAmmoniaPdHydrogenation

Xiaokang Chen、Shengliang Zhai、Yi Tan、Le Su、Dong Zhai、Wei-Qiao Deng、Hao Wu

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Institute of Frontier Chemistry,School of Chemistry and Chemical Engineering,Shandong University,Qingdao 266071,Shandong,China

College of Physics and Information Engineering,Shanxi Normal University,Taiyuan 030031,Shanxi,China

Suzhou Research Institute of Shandong University,Suzhou 215123,Jiangsu,China

National Key R&D Program of ChinaNational Key R&D Program of ChinaNatural Science Foundation of Shandong ProvinceNatural Science Foundation of Jiangsu ProvinceTaishan Scholars ProjectQilu Young Scholars Program of Shandong University

2022YFA15031042022YFA15031022022HWYQ-009BK20230243tspd20230601

2024

10.1016/j.jechem.2024.05.001

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.96(9)