A novel bimetal cluster [AuCu(SR)](PPh) (SR = 2,4-dichlorothiophenol) has been successfully synthesized, which can be viewed as a Au@Au core and four trimeric Cu(SR) staples. Compared to monometallic Au(TBBT) and Cu(CHT)(PPh) clusters, the [AuCu(CHClS)](PPh) cluster has much higher catalytic efficiency for nitrate electroreduction to ammonia.
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http://dx.doi.org/10.1039/d4cc02085e | DOI Listing |
Nat Mater
January 2025
Department of Interface Science, Fritz-Haber Institute of the Max-Planck Society, Berlin, Germany.
Electrocatalysts alter their structure and composition during reaction, which can in turn create new active/selective phases. Identifying these changes is crucial for determining how morphology controls catalytic properties but the mechanisms by which operating conditions shape the catalyst's working state are not yet fully understood. In this study, we show using correlated operando microscopy and spectroscopy that as well-defined CuO cubes evolve under electrochemical nitrate reduction reaction conditions, distinct catalyst motifs are formed depending on the applied potential and the chemical environment.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Institute of Chemistry Chinese Academy of Sciences, Institute of chemistry, Beiyijie number 2, Zhongguancun, 100190, Beijing, CHINA.
Electrocatalytic nitrate reduction reaction (NO3RR) in alkaline electrolyte presents a sustainable pathway for energy storage and green ammonia (NH3) synthesis. However, it remains challenging to obtain high activity and selectivity due to the limited protonation and/or desorption processes of key intermediates. Herein, we propose a strategy to regulate the acid hardness nature of Cu catalyst by introducing appropriate modifier.
View Article and Find Full Text PDFACS Nano
January 2025
Key Laboratory of Mesoscopic Chemistry of MOE and Jiangsu Provincial Laboratory of Nanotechnology, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
Ammonia synthesis via nitrate electroreduction is more attractive and sustainable than the energy-extensive Haber-Bosch process and intrinsically sluggish nitrogen electroreduction. Herein, we have designed a single-site Cu catalyst on hierarchical nitrogen-doped carbon nanocage support (Cu/hNCNC) for nitrate electroreduction, which achieves an ultrahigh ammonia yield rate (YR) of 99.4 mol h g (2.
View Article and Find Full Text PDFInorg Chem
January 2025
Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, MOE Key Laboratory of New Processing Technology for Nonferrous Metals and Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, Guangxi, China.
Here, we reported a highly efficient nitrate electroreduction (NORR) electrocatalyst that integrated alloying and heterostructuring strategies comprising FeCo alloy and MoN (FeCo-MoN/NC). Notably, the maximum NH Faraday efficiency (FE) of 83.24%, NH yield of 12.
View Article and Find Full Text PDFAdv Mater
January 2025
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
Nitrate electroreduction is promising for achieving effluent waste-water treatment and ammonia production with respect to the global nitrogen balance. However, due to the impeded hydrogenation process, high overpotentials need to be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy is developed to optimize the interfacial HO behavior for accelerating the hydrogenation conversion of nitrate to ammonia at ultralow overpotentials.
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