Pd Nanoparticle Size-Dependent H* Coverage for Cu-Catalyzed Nitrate Electro-Reduction to Ammonia in Neutral Electrolyte

Zhu, Hongbo1,2; Wang, Jiacheng Jayden3; Xu, Zian4; Tan, Yongwen2; Wang, Jiacheng1

2024-08-01

10.1002/smll.202404919

SMALL   影响因子和分区

1613-6810

1613-6829

Electrochemical conversion of nitrate (NO3-) to ammonia (NH3) is an effective approach to reduce nitrate pollutants in the environment and also a promising low-temperature, low-pressure method for ammonia synthesis. However, adequate H* intermediates are highly expected for NO3- hydrogenation, while suppressing competitive hydrogen evolution. Herein, the effect of H* coverage on the NO3RR for ammonia synthesis by Cu electrocatalysts is investigated. The H* coverage can be adjusted by changing Pd nanoparticle sizes. The optimized Pd@Cu with an average Pd size of 2.88 nm shows the best activity for NO3RR, achieving a maximum Faradaic efficiency of 97% (at -0.8 V vs RHE) and an NH3 yield of 21 mg h(-1) cm(-2), from an industrial wastewater level of 500 ppm NO3-. In situ electrochemical experiments indicate that Pd particles with 2.88 nm can promote NO3- hydrogenation to NH3 via well-modulated coverage of adsorbed H* species. Coupling the anodic glycerol oxidation reaction, ammonium and formate are successfully obtained as value-added products in a membrane electrode assembly electrolyzer. This work provides a feasible strategy for obtaining size-dependent H* intermediates for hydrogenation.

ammonia synthesis electrochemical nitrate reduction H* coverage membrane electrode assembly electrolyzer Pd nanoparticles

SCI ; EI

英语

其他

National Natural Science Foundation of China[52072389] ; Science and Technology Commission of Shanghai Municipality["22DZ1205600","20520760900"] ; Program of Shanghai Academic Research Leader[20XD1424300]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:001283054900001

WILEY-V C H VERLAG GMBH

Web of Science

1.Taizhou Univ, Inst Electrochem, Sch Mat Sci & Engn, Zhejiang Key Lab Isl Green Energy & New Mat, Taizhou 318000, Peoples R China
2.Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Peoples R China
3.Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine M, Shanghai 200050, Peoples R China
4.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China

Zhu, Hongbo,Wang, Jiacheng Jayden,Xu, Zian,et al. Pd Nanoparticle Size-Dependent H* Coverage for Cu-Catalyzed Nitrate Electro-Reduction to Ammonia in Neutral Electrolyte[J]. SMALL,2024.

Zhu, Hongbo,Wang, Jiacheng Jayden,Xu, Zian,Tan, Yongwen,&Wang, Jiacheng.(2024).Pd Nanoparticle Size-Dependent H* Coverage for Cu-Catalyzed Nitrate Electro-Reduction to Ammonia in Neutral Electrolyte.SMALL.

Zhu, Hongbo,et al."Pd Nanoparticle Size-Dependent H* Coverage for Cu-Catalyzed Nitrate Electro-Reduction to Ammonia in Neutral Electrolyte".SMALL (2024).