Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide

Sun，Huachuan1; Li，Linfeng1; Chen，Hsiao Chien2,3; Duan，Delong4; Humayun，Muhammad1; Qiu，Yang5; Zhang，Xia6; Ao，Xiang1; Wu，Ying6; Pang，Yuanjie1; Huo，Kaifu1; Wang，Chundong1; Xiong，Yujie4

2022

10.1016/j.scib.2022.08.008

Science Bulletin   影响因子和分区

2095-9273

2095-9281

Anodic urea oxidation reaction (UOR) is an intriguing half reaction that can replace oxygen evolution reaction (OER) and work together with hydrogen evolution reaction (HER) toward simultaneous hydrogen fuel generation and urea-rich wastewater purification; however, it remains a challenge to achieve overall urea electrolysis with high efficiency. Herein, we report a multifunctional electrocatalyst termed as Rh/NiV-LDH, through integration of nickel-vanadium layered double hydroxide (LDH) with rhodium single-atom catalyst (SAC), to achieve this goal. The electrocatalyst delivers high HER mass activity of 0.262 A mg and exceptionally high turnover frequency (TOF) of 2.125 s at an overpotential of 100 mV. Moreover, exceptional activity toward urea oxidation is addressed, which requires a potential of 1.33 V to yield 10 mA cm, endorsing the potential to surmount the sluggish OER. The splendid catalytic activity is enabled by the synergy of the NiV-LDH support and the atomically dispersed Rh sites (located on the Ni-V hollow sites) as evidenced both experimentally and theoretically. The self-supported Rh/NiV-LDH catalyst serving as the anode and cathode for overall urea electrolysis (1 mol L KOH with 0.33 mol L urea as electrolyte) only requires a small voltage of 1.47 V to deliver 100 mA cm with excellent stability. This work provides important insights into multifunctional SAC design from the perspective of support sites toward overall electrolysis applications.

High turnover frequency Hydrogen evolution reaction Layer double hydroxide Overall urea electrolysis Single-atomically active centers

SCI ; EI

英语

ESI高被引

其他

National Key R&D Pro-gram of China[2017YFE0120500] ; National Natural Science Foundation of China["51972129","51702150","21725102"] ; Key Research and Development Program of Hubei[2020BAB079] ; Bintuan Science and Technology Program["2020DB002","2022DB009"] ; Science and Technology Innovation Committee Foundation of Shenzhen["JCYJ20210324141613032","JCYJ20190809142019365"]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000862291100013

ELSEVIER

20223312577394

Anodic oxidation ; Catalyst activity ; Electrocatalysts ; Electrodes ; Electrolysis ; Electrolytes ; Hydrogen production ; Metabolism ; Nickel compounds ; Potassium hydroxide ; Purification ; Vanadium compounds

Gas Fuels:522 ; Protection Methods:539.2.1 ; Electric Batteries and Fuel Cells:702 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2

2-s2.0-85136751542

Scopus

1.School of Optical and Electronic Information,Wuhan National Laboratory for Optoelectronics,Optics Valley Laboratory,Huazhong University of Science and Technology,Wuhan,430074,China
2.Center for Reliability Science and Technologies,Chang Gung University,Taoyuan,33302,China
3.Kidney Research Center,Department of Nephrology,Chang Gung Memorial Hospital,Linkou,Taoyuan,33305,China
4.School of Chemistry and Materials Science,University of Science and Technology of China,Hefei,230026,China
5.Pico Center,SUSTech Core Research Facilities,Southern University of Science and Technology,Shenzhen,518055,China
6.College of Chemistry and Chemical Engineering,Tarim University,Alaer,843300,China

Sun，Huachuan,Li，Linfeng,Chen，Hsiao Chien,et al. Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide[J]. Science Bulletin,2022,67(17):1763-1775.

Sun，Huachuan.,Li，Linfeng.,Chen，Hsiao Chien.,Duan，Delong.,Humayun，Muhammad.,...&Xiong，Yujie.(2022).Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide.Science Bulletin,67(17),1763-1775.

Sun，Huachuan,et al."Highly efficient overall urea electrolysis via single-atomically active centers on layered double hydroxide".Science Bulletin 67.17(2022):1763-1775.