Article
Chemistry, Applied
Xudong Lv, Junyan Liu, Tao Shao, Meng Ye, Shengwei Liu
Summary: In this study, atomic-dispersed Sn-modified Cu nanowires (Cu@Sn NWs) were synthesized for selective electrocatalytic CO2 reduction reaction (CO2RR) to CO with an optimized FECO of 96.4%. Moreover, the formaldehyde oxidation half-reaction (FOR) at MnO2/CP anode was introduced to build a novel CO2RR/FOR system, further improving CO2RR efficiency and reducing energy consumption. Compared with the CO2RR/WOR system, the CO2RR/FOR system showed higher CO2RR performance and tunable selectivity of converting formaldehyde to formic acid. Furthermore, the working cell voltage and energy consumption could be significantly reduced over the CO2RR/FOR system, compared to the CO2RR/WOR system.
Article
Nanoscience & Nanotechnology
Rik V. Mom, Luis-Ernesto Sandoval-Diaz, Dunfeng Gao, Cheng-Hao Chuang, Emilia A. Carbonio, Travis E. Jones, Rosa Arrigo, Danail Ivanov, Michael Haevecker, Beatriz Roldan Cuenya, Robert Schloegl, Thomas Lunkenbein, Axel Knop-Gericke, Juan-Jesus Velasco-Velez
Summary: Catalyst degradation and product selectivity changes are significant challenges in the electrochemical reduction of CO2 on copper electrodes. In this study, the long-term evolution of Cu nanosized crystals during the CO2 reduction reaction was investigated using in situ X-ray spectroscopy, in situ electron microscopy, and ex situ characterization techniques. The electronic structure of the electrode remained unchanged under cathodic potentiostatic control, while the electrode morphology was modified by prolonged CO2 electroreduction. These morphological changes led to increased current and a shift in product selectivity from value-added hydrocarbons to less valuable side reaction products. Overall, our results indicate the importance of stabilizing a faceted Cu morphology for optimal long-term performance in the selective reduction of CO2 into hydrocarbons and oxygenated products.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Bing Wei, Yusong Xiong, Zhengyuan Zhang, Jinhui Hao, Longhua Li, Weidong Shi
Summary: This study successfully prepared bimetallic InxCuy nanoparticles catalysts, which raised the Faraday efficiency of formic acid by In-based materials by adjusting the growth direction of the catalyst crystal facets.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Xinyue Wang, Yu Wang, Xiahan Sang, Wanzhen Zheng, Shihan Zhang, Ling Shuai, Bin Yang, Zhongjian Li, Jianmeng Chen, Lecheng Lei, Nadia Mohd Adli, Michael K. H. Leung, Ming Qiu, Gang Wu, Yang Hou
Summary: An axial traction strategy was developed to optimize the electronic structure of the M-N-4 moiety, leading to atomically dispersed nickel sites coordinated with four nitrogen atoms and one axial oxygen atom embedded within the carbon matrix (Ni-N-4-O/C). This Ni-N-4-O/C electrocatalyst exhibited excellent CO2RR performance with a high CO Faradic efficiency close to 100% at -0.9 V, maintaining the CO FE above 90% in a wide potential window. The superior CO2RR activity is attributed to the axial traction effect induced by the Ni-N-4-O active moiety.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Justus S. Diercks, Juan Herranz, Maximilian Georgi, Natasa Diklic, Piyush Chauhan, Kathrin Ebner, Adam H. Clark, Maarten Nachtegaal, Alexander Eychmuller, Thomas J. Schmidt
Summary: Palladium is an electrocatalyst that can selectively generate carbon monoxide or formate at high and low overpotentials, respectively. Previous studies have been inconclusive about palladium's ability to form a hydride phase and its effect on CO2 reduction reaction (CO2RR) selectivity. This study used electrochemical measurements and in situ X-ray absorption spectroscopy to reveal the strong influence of adsorbed CO on the formation rate of Pd-hydride, and confirmed the complete formation of beta-phase PdHx at all applied potentials under CO2RR conditions.
Article
Chemistry, Multidisciplinary
Shenghua Chen, Bingqing Wang, Jiexin Zhu, Liqiang Wang, Honghui Ou, Zedong Zhang, Xiao Liang, Lirong Zheng, Liang Zhou, Ya-Qiong Su, Dingsheng Wang, Yadong Li
Summary: A single-atomic Cu catalyst supported by Lewis acid on metal oxides was designed for efficient electrocatalytic CO2 reduction to CH4, achieving a Faradaic efficiency of 62% at -1.2 V (vs RHE) with a current density of 153.0 mA cm(-2).
Article
Chemistry, Physical
Huaxin Li, Xian Yue, Yunsheng Qiu, Zhou Xiao, Xianbo Yu, Chao Xue, Junhui Xiang
Summary: A series of novel CuxSny bimetallic alloy catalysts were designed for electrocatalytic CO2RR to HCOOH generation, with Cu1Sn3-CC catalyst demonstrating high selectivity and Faradaic efficiency for HCOOH evolution, as well as a low onset potential and high maximum current density. Furthermore, the catalyst maintained a Faraday efficiency higher than 88.35% after long-term operation.
MATERIALS TODAY ENERGY
(2021)
Article
Chemistry, Physical
Arnaud Thevenon, Alonso Rosas-Hernandez, Alex M. Fontani Herreros, Theodor Agapie, Jonas C. Peters
Summary: Selective conversion of CO2 to CO with high Faradaic efficiencies (>99%) on planar silver electrodes was achieved using simple pyridinium-based additives, which form organic films altering CO2RR selectivity. Electrochemical kinetic and mechanistic data suggest that a hydrophobic organic layer inhibits hydrogen production selectively by limiting proton mass transport, while pointing to proton transfer as the rate-determining step instead of electron transfer for planar Ag electrodes.
Article
Chemistry, Physical
Diego Gianolio, Michael D. Higham, Matthew G. Quesne, Matteo Aramini, Ruoyu Xu, Alex I. Large, Georg Held, Juan-Jesus Velasco-Velez, Michael Haevecker, Axel Knop-Gericke, Chiara Genovese, Claudio Ampelli, Manfred Erwin Schuster, Siglinda Perathoner, Gabriele Centi, C. Richard A. Catlow, Rosa Arrigo
Summary: Operando soft and hard X-ray spectroscopic techniques were used to investigate Zn-containing Cu nanostructured electrocatalysts in CO2 hydrogenation reaction. The study reveals that Zn is alloyed with Cu in the bulk of the nanoparticles, while low reducible Cu(I)-O species are consumed at the interface. The Cu-Zn system represents the optimal active ensembles with stabilized Cu(I)-O, which activates CO2 and supplies H atoms for the hydrogenation reaction.
Article
Chemistry, Physical
Zhiming Wei, Jie Ding, Xinxuan Duan, Guan-Lin Chen, Feng-Yi Wu, Li Zhang, Xiaoju Yang, Qiao Zhang, Qinye He, Zhaoyang Chen, Jian Huang, Sung-Fu Hung, Xuan Yang, Yueming Zhai
Summary: Heteroatom-doped Cu-based catalysts not only exhibit enhanced activity of CO2 reduction reaction (CO2RR), but also have the potential to control the selectivity of CO2RR. However, it is challenging to identify the origin of the improved performance due to the complex nature of Cu-based materials, impeding the rational design of catalysts. This research demonstrates that the activity and selectivity of CO2RR can be adjusted by manipulating the lattice strain of Cu-based catalysts. The study combines spectroscopic characterizations, operando and ex situ, to reveal the transformation of Sndoped CuO catalysts from compressively strained to tensile-strained Sn/Cu alloy catalysts under reaction conditions.
Article
Electrochemistry
Yuting Liu, Hua Liu, Cheng Wang, Yali Wang, Jiaxing Lu, Huan Wang
Summary: In this study, Cu/Cu2O(X) catalysts (where X = I, Br, Cl) were reconstructed via cyclic voltammetry on carbon paper for selective electroreduction of CO2 to produce multicarbon products (C2+). The Cu/Cu2O(Cl), Cu/Cu2O(Br), and Cu/Cu2O(I) catalysts achieved Faradaic efficiencies (FE) of 31%, 34%, and 58%, respectively, for C2+ (C2H4, C2H5OH, C3H8OH) production at a potential of -0.76 V vs. the reversible hydrogen electrode (RHE). The Cu+ and Cu0 species obtained from the reconstruction of Cu/CuX are primarily responsible for the high C2+ producing activity.
ELECTROCHEMISTRY COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Bupmo Kim, Dayoung Kwon, Jin-Ook Baeg, P. Muthu Austeria, Geun Ho Gu, Jeong-Hyeon Lee, Jeehun Jeong, Wooyul Kim, Wonyong Choi
Summary: A new single-atom dual-atom-site catalyst has been developed to significantly promote the production of formaldehyde through the four-electron transfer pathway of *OCHO. The neighboring Sn(II)-Cu(I) dual-atom sites stabilize the intermediates for formaldehyde production, and the adsorbed *HCHO intermediate is detected by in situ Fourier transform infrared spectroscopy. This study provides a unique example of controlling the selectivity of multi-electron transfer mechanisms for CO2 photoconversion using a heteronuclear dual-atom-site catalyst to generate an uncommon product (formaldehyde) from CO2 reduction.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zedong Zhang, Shenghua Chen, Jiexin Zhu, Chenliang Ye, Yu Mao, Bingqing Wang, Gang Zhou, Liqiang Mai, Ziyun Wang, Xiangwen Liu, Dingsheng Wang
Summary: In this work, a Pd delta--Cu3N catalyst containing charge-separated Pd delta--Cu delta+ atom pair is designed to stabilize the Cu delta+ sites and promote the CO dimerization process. The achieved 14-fold increase in C2 product Faradaic efficiency demonstrates the effectiveness of this strategy for enhancing CO2 RR.
Article
Materials Science, Multidisciplinary
Shengnan Wang, Dan Wang, Benqiang Tian, Xiangxiang Gao, Lu Han, Yang Zhong, Shuchang Song, Zhili Wang, Yaping Li, Jianing Gui, Marshet G. Sendeku, Ying Zhang, Yun Kuang, Xiaoming Sun
Summary: The study reveals the synergistic role of Cu+ and Cu-0 species in Cu2O-Cu interfaces through density functional theory calculations, which leads to low free energy of *COCO intermediate formation and H2O dissociation, promoting high selectivity towards multi-carbon products. Guided by these results, an oxide-derived copper electrode activation strategy is designed to build synergistic Cu+ and Cu-0 on Cu2O-Cu interfaces, resulting in superior Faradaic efficiencies for C2H4 and C2+ products compared to Cu2O cubes. This study demonstrates the importance of Cu-0 and Cu+ synergy in improving the selectivity of valuable multi-carbon products in electrocatalytic CO2 conversion.
SCIENCE CHINA-MATERIALS
(2023)
Article
Chemistry, Analytical
Cheng-Jie Jiang, Yue Hou, Hua Liu, Le-Ting Wang, Gui-Rong Zhang, Jia-Xing Lu, Huan Wang
Summary: In this study, Cu nanoparticles loaded on nitrogen-doped carbon materials were prepared for the electrochemical reduction of CO2, showing good selectivity for C1 and significant catalytic activity.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Article
Electrochemistry
Jack H. Baricuatro, Youn-Geun Kim, Carol L. Korzeniewski, Manuel P. Soriaga
ELECTROCHEMISTRY COMMUNICATIONS
(2018)
Article
Chemistry, Physical
Youn-Geun Kim, Jack H. Baricuatro, Manuel P. Soriaga
Article
Electrochemistry
Sheng Shen, Xiaoyue Zhang, Syed Mubeen, Manuel P. Soriaga, John L. Stickney
ELECTROCHIMICA ACTA
(2019)
Article
Chemistry, Analytical
Jack H. Baricuatro, Youn-Geun Kim, Chu F. Tsang, Alnald C. Javier, Kyle D. Cummins, John C. Hemminger
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2020)
Article
Chemistry, Applied
Jack H. Baricuatro, Youn-Geun Kim, Carol L. Korzeniewski, Manuel P. Soriaga
Article
Chemistry, Multidisciplinary
Michelle Duran-Chaves, Jean Sanabria Chinchilla
JOURNAL OF CHEMICAL EDUCATION
(2020)
Article
Chemistry, Analytical
Jack H. Baricuatro, Youn-Geun Kim, Chu F. Tsang, Alnald C. Javier, Kyle D. Cummins, John C. Hemminger
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2020)
Article
Chemistry, Physical
Jack H. Baricuatro, Soonho Kwon, Youn-Geun Kim, Kyle D. Cummins, Saber Naserifar, William A. Goddard
Summary: The electrochemical reduction of CO2 to value-added products is an attractive strategy to address the increasing atmospheric CO2 concentration. Copper is known as the only pure metal catalyst that can convert CO2 to oxygenates and hydrocarbons, but its efficiencies and potentials are not optimal. Through in silico strategies and experimental validation, it has been shown that the surface coverages of H*, OH*, and CO* on Cu(100) can predict the shift in the nu(CO) as a function of potential and pH, providing a theoretical foundation for predicting catalyst performance.
Article
Chemistry, Physical
Soonho Kwon, Youn-Geun Kim, Jack H. Baricuatro, William A. Goddard
Summary: The systematic investigation of CO2 reduction on Cu(100) surfaces revealed a dramatic change in step-edge direction upon adsorption and desorption of CO at specific potentials, as observed by operando electrochemical scanning tunneling microscopy.
Article
Electrochemistry
Javier E. Rodriguez-Yanez, Sebastian Feliu Batlle, Jean Sanabria-Chinchilla, Jose Felix Rojas-Marin
Summary: The corrosion level in tropical atmospheric conditions in Central America and The Caribbean is influenced by the exposure angle and the sample's orientation. The study shows a decrease in corrosion with increasing angle and variations in corrosion levels between different sides of the sample. Both classical and electrochemical methods provided consistent results.
ELECTROCHIMICA ACTA
(2023)
Article
Electrochemistry
Chu F. Tsang, Alnald C. Javier, Youn-Geun Kim, Jack H. Baricuatro, Kyle D. Cummins, Jutae Kim, Gregory Jerkiewicz, John C. Hemminger, Manuel P. Soriaga
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2018)
