Article
Chemistry, Multidisciplinary
Ruoqi Liu, Ting Guo, Hao Fei, Zhuangzhi Wu, Dezhi Wang, Fangyang Liu
Summary: In this study, different active sites of MoS2 were found to exhibit different catalytic selectivity for nitrogen reduction and hydrogen evolution reactions through DFT calculations. A new synergistic mechanism was proposed and a self-sacrificial strategy using g-C3N4 as templates was developed to synthesize 1T-MoS2 with an ultrahigh 1T content. This work provides a promising new direction for synchronizing selectivity and activity in multistep catalytic reactions.
Article
Chemistry, Physical
Yu-Han Tseng, Kai-Yuan Hsiao, Chong-Chi Chi, Ming-Yen Lu
Summary: The NRR activity can be enhanced by using Fe/Co co-doped MoS2 nanosheets as electrocatalysts, resulting in improved NH3 yield rate and Faradaic efficiency. Density functional theory calculations reveal the superior electrocatalytic activity of FeCo-MoS2 nanosheets.
MATERIALS TODAY ENERGY
(2023)
Article
Chemistry, Physical
Benjamin P. Charnay, Zhihao Cui, Melissa A. Marx, Joseph Palazzo, Anne C. Co
Summary: This study investigates the electrochemical reduction of aldehydes to alcohols as a pathway for converting CO2 to alcohols. Experimental results support the proposed mechanism of reducing acetaldehyde and propionaldehyde to ethanol and 1-propanol on a Cu catalyst. Notably, acetaldehyde is selectively reduced to ethanol on Cu, but not on Au, as supported by both experimental observations and DFT calculations.
Review
Nanoscience & Nanotechnology
Junjun Li, Sulaiman Umar Abbas, Haiqing Wang, Zhicheng Zhang, Wenping Hu
Summary: Electrocatalytic CO2 reduction reaction is crucial for storing and transforming renewable energy into chemical energy. Interface engineering has emerged as an effective strategy to modulate electrocatalytic performance by controlling local reactant concentration and achieving desirable reaction pathways, inhibiting competing hydrogen generation, and promoting CO2 mass transfer. Opportunities and challenges of interface engineering for CO2RR are also discussed.
NANO-MICRO LETTERS
(2021)
Article
Chemistry, Physical
Hao Fei, Ting Guo, Yue Xin, Liangbing Wang, Ruoqi Liu, Dezhi Wang, Fangyang Liu, Zhuangzhi Wu
Summary: Sulfur vacancy-rich MoS2 doped with P shows great potential as an excellent electrocatalyst for NRR. P-M-1 achieved high NH3 yield rate and NRR efficiency through the creation of sulfur vacancies as active centers and modulation of electronic structure.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Leily Majidi, Alireza Ahmadiparidari, Nannan Shan, Saurabh N. Misal, Khagesh Kumar, Zhehao Huang, Sina Rastegar, Zahra Hemmat, Xiaodong Zou, Peter Zapol, Jordi Cabana, Larry A. Curtiss, Amin Salehi-Khojin
Summary: A 2D copper-based conductive MOF, Cu-THQ, exhibits excellent catalytic activity for aqueous CO2 reduction reaction (CO2RR) with low overpotentials. The material shows high CO production rate and current density at low overpotentials, making it a promising candidate for practical applications in CO2RR.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Zhong Liang, Lianpeng Song, Yong Jiang, Jincheng Liu, Yabin Zhang, Qian Zhang, Chun-Hua Yan, Yaping Du
Summary: This work presents the synthesis and characterization of a rare earth-based single-atom combo catalyst BiY/CN for electrochemical reduction of CO2 to formic acid. The experimental results show that the Y sites in the catalyst, covered by hydroxyls, not only avoid poisoning but also affect the charge state of Bi sites, promoting catalytic performance.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Bishnubasu Giri, Arup Mahata, Tatinaidu Kella, Debaprasad Shee, Filippo De Angelis, Somnath Maji
Summary: The introduction of tetrazole moiety into the ligand framework of isomeric ruthenium catalysts has altered the catalytic pathway for the electrochemical reduction of CO2 to CO, resulting in significantly lower over-potential and the formation of a metallocarboxylate intermediate. The mechanism follows the ECE pathway and has been supported by various characterization techniques and theoretical studies.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Tian-Wen Jiang, Ya-Wei Zhou, Xian-Yin Ma, Xianxian Qin, Hong Li, Chen Ding, Bei Jiang, Kun Jiang, Wen-Bin Cai
Summary: The study investigates the mechanism of CO2RR on Pd and Pd-B film electrodes using various analytical techniques, demonstrating the role of surface CO and the influence of B-doping on CO2RR at different potentials.
Article
Chemistry, Multidisciplinary
Hao Zhang, Zhiqiang Wang, Chenglong Ma, Zhenhua Zhou, Limei Cao, Xueqing Gong, Chunxiao Dong, Ji Yang
Summary: A high-performance non-precious metal-based cathode catalyst was successfully developed using a soft-template route, exhibiting higher diffusion-limiting current density compared to a commercial Pt/C catalyst. This catalyst showed lattice shrinking phenomenon and increased occupancy of e(g) orbitals, enhancing its intrinsic activity.
Article
Chemistry, Physical
Yu Zhang, Luca Mascaretti, Michele Melchionna, Olivier Henrotte, Stepan Kment, Paolo Fornasiero, Alberto Naldoni
Summary: A fabrication approach was developed to create TiN/F-doped carbon hybrids with high catalytic activity for H2O2 production. These hybrids showed a maximum H2O2 selectivity of 90% and achieved a H2O2 productivity of 207 mmol g(TiN) (-1) h(-1) at 0.2 V vs RHE. The formation of nanocomposites played a key role in achieving high currents, with increased TiO x N y surface content promoting higher H(2)O(2) selectivity and fluorinated nanocarbon imparting good stability to the electrodes due to their superhydrophobic properties.
Article
Chemistry, Physical
Debolina Misra, Giovanni Di Liberto, Gianfranco Pacchioni
Summary: The electrochemical reduction of CO2 on single atom catalysts (SAC) is a promising but complex process that requires a deep understanding of each step. Most theoretical studies neglect important effects such as the site's capability to bind and activate CO2, competing reaction paths via intermediate isomer formation, and the role of water. Our research shows that these aspects are crucial for CO2 reduction.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Ziyang Wei, Philippe Sautet
Summary: Copper is the most important catalyst for the carbon dioxide reduction reaction (CO2RR), but traditional methods have difficulties in studying the mechanism. This study used a more accurate method to investigate the CO2RR mechanism on Cu(100) facet.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Zheng Zhang, Xin Huang, Zhou Chen, Junjiang Zhu, Balazs Endrodi, Csaba Janaky, Dehui Deng
Summary: Electrocatalytic CO2 reduction reaction (CO2RR) in membrane electrode assembly (MEA) systems is a promising technology due to the direct transport of gaseous CO2 to the cathode catalyst layer and the absence of liquid electrolyte between the cathode and the anode. Recent progress has shown the way to achieve industrially relevant performance. This review focuses on the principles of CO2RR in MEA, particularly the gas diffusion electrodes and ion exchange membranes, as well as the anode processes and voltage distribution. The generation of different reduced products and corresponding catalysts is summarized, and the challenges and opportunities for future research are highlighted.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Shan Jiang, Luca D'Amario, Holger Dau
Summary: Copper electrodes have shown excellent catalytic performance in the reduction of CO2, but the underlying reasons are not well understood. In this study, using operando Raman experiments, the researchers investigated the structures and molecular interactions at the electrode-electrolyte interface and discovered the formation of a copper carbonate hydroxide (CuCarHyd) that resembles malachite. It was found that the reduction of carbonate ions, bound to the metallic Cu electrode in the form of CuCarHyd structures, was the starting point of carbon reduction, challenging previous mechanistic models. The presence of CuCarHyd patches at catalytic potentials could be attributed to alkalization and local electrical potential gradients. These findings provide important insights into improving the efficiency of CO2 reduction reactions and understanding their mechanisms.
Article
Chemistry, Multidisciplinary
Ning Wang, Pengfei Ou, Sung-Fu Hung, Jianan Erick Huang, Adnan Ozden, Jehad Abed, Ivan Grigioni, Clark Chen, Rui Kai Miao, Yu Yan, Jinqiang Zhang, Ziyun Wang, Roham Dorakhan, Ahmed Badreldin, Ahmed Abdel-Wahab, David Sinton, Yongchang Liu, Hongyan Liang, Edward H. Sargent
Summary: Direct electrolysis of pH-neutral seawater to generate hydrogen faces an anodic competition issue between the chlorine evolution and the oxygen evolution reaction (OER), resulting in low current density and limited operating stability. In this study, a proton-adsorption-promoting strategy has been proposed to increase the OER rate, allowing for enhanced and stable neutral seawater splitting. Palladium-doped cobalt oxide (Co3-xPdxO4) catalysts exhibit the best performance with an OER overpotential of 370 mV at 10 mA cm(-2) in pH-neutral simulated seawater, outperforming Co3O4 by 70 mV. Co3-xPdxO4 catalysts also demonstrate long-term stability in neutral seawater, with 450 hours at 200 mA cm(-2) and 20 hours at 1 A cm(-2). Experimental and theoretical analyses suggest that the inclusion of SPA cations accelerates the rate-determining water dissociation step in the neutral OER pathway, while ruling out additional OER sites as a main factor.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Mingchuan Luo, Adnan Ozden, Ziyun Wang, Fengwang Li, Jianan Erick Huang, Sung-Fu Hung, Yuhang Wang, Jun Li, Dae-Hyun Nam, Yuguang C. Li, Yi Xu, Ruihu Lu, Shuzhen Zhang, Yanwei Lum, Yang Ren, Longlong Fan, Fei Wang, Hui-hui Li, Dominique Appadoo, Cao-Thang Dinh, Yuan Liu, Bin Chen, Joshua Wicks, Haijie Chen, David Sinton, Edward H. Sargent
Summary: Upgrading carbon dioxide/monoxide to multi-carbon C2+ products using renewable electricity offers a sustainable approach to fuel and chemical production. A new coordination polymer catalyst consisting of Cu(I) and benzimidazole units linked via Cu(I)-imidazole coordination bonds enables selective reduction of CO to acetate with a 61% Faradaic efficiency. The catalyst integrated in a cation exchange membrane-based membrane electrode assembly allows stable acetate electrosynthesis and achieves concentrated acetate collection, high CO-to-acetate conversion efficiency, and good acetate full-cell energy efficiency.
ADVANCED MATERIALS
(2023)
Article
Multidisciplinary Sciences
Hao Chen, Aidan Maxwell, Chongwen Li, Sam Teale, Bin Chen, Tong Zhu, Esma Ugur, George Harrison, Luke Grater, Junke Wang, Zaiwei Wang, Lewei Zeng, So Min Park, Lei Chen, Peter Serles, Rasha Abbas Awni, Biwas Subedi, Xiaopeng Zheng, Chuanxiao Xiao, Nikolas J. Podraza, Tobin Filleter, Cheng Liu, Yi Yang, Joseph M. Luther, Stefaan De Wolf, Mercouri G. Kanatzidis, Yanfa Yan, Edward H. Sargent
Summary: The open-circuit voltage deficit in wide-bandgap perovskite solar cells is larger than in perovskites with a bandgap of approximately 1.5 eV. The limiting factor for the open-circuit voltage is found to be recombination at the electron-transport-layer contact, resulting from inhomogeneous surface potential and poor energetic alignment. To address this issue, a new surface treatment using diammonium molecules is introduced to achieve a more uniform distribution of surface potential.
Article
Chemistry, Multidisciplinary
Ning Wang, Pengfei Ou, Rui Kai Miao, Yuxin Chang, Ziyun Wang, Sung-Fu Hung, Jehad Abed, Adnan Ozden, Hsuan-Yu Chen, Heng-Liang Wu, Jianan Erick Huang, Daojin Zhou, Weiyan Ni, Lizhou Fan, Yu Yan, Tao Peng, David Sinton, Yongchang Liu, Hongyan Liang, Edward H. Sargent
Summary: Acidic water electrolysis is used to produce hydrogen for chemical and fuel applications. Doping Ba cations into a Co3O4 framework promotes the oxide path mechanism and improves activity in acidic electrolytes, leading to more efficient water oxidation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Pawan Kumar, Karthick Kannimuthu, Ali Shayesteh Zeraati, Soumyabrata Roy, Xiao Wang, Xiyang Wang, Subhajyoti Samanta, Kristen A. Miller, Maria Molina, Dhwanil Trivedi, Jehad Abed, Astrid Campos Mata, Hasan Al-Mahayni, Jonas Baltrusaitis, George Shimizu, Yimin A. Wu, Ali Seifitokaldani, Edward H. Sargent, Pulickel M. Ajayan, Jinguang Hu, Md Golam Kibria
Summary: This study presents a macromolecule-assisted synthesis approach for single atom catalysts (SACs) that allows for the production of high-density cobalt single atoms with exceptional catalytic properties. The resulting SACs, embedded within a highly porous carbon network, exhibited significantly enhanced electrocatalytic activity for the oxygen evolution reaction (OER), with long-term stability. Experimental and theoretical results provide valuable insights into the mechanisms underlying the improved catalytic performance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ya-Kun Wang, Haoyue Wan, Jian Xu, Yun Zhong, Eui Dae Jung, So Min Park, Sam Teale, Muhammad Imran, You-Jun Yu, Pan Xia, Yu-Ho Won, Kwang-Hee Kim, Zheng-Hong Lu, Liang-Sheng Liao, Sjoerd Hoogland, Edward H. Sargent
Summary: Researchers have developed a bifunctional ETL (CNT2T) to address the issues caused by the electron-transporting layer (ETL) in red InP LEDs, resulting in significantly improved efficiency and brightness of the devices.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Electrochemistry
Amanda F. Baxter, Jehad Abed, Daniela V. Fraga V. Alvarez, Daojin Zhou, Dhruti Kuvar, Edward H. Sargent, Daniel V. Esposito
Summary: In this study, RuO2 nanoparticles were encapsulated with semipermeable, nanoscopic SiOx overlayers to improve their stability. The best-performing SiOx|RuO2 electrodes consisted of 2-3 nm thick SiOx overlayers on top of RuO2 particles. These electrodes exhibited lower overpotentials and demonstrated an ability to retain OER activity over time.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Sasa Wang, Asif Abdullah Khan, Sam Teale, Jian Xu, Darshan H. Parmar, Ruyan Zhao, Luke Grater, Peter Serles, Yu Zou, Tobin Filleter, Dwight S. Seferos, Dayan Ban, Edward H. Sargent
Summary: Piezoelectric materials are essential for self-powered electronics and energy harvesting. However, existing piezoelectrics have limitations in terms of charge and voltage coefficients. In this study, researchers developed a molecular piezoelectric material with enhanced properties by utilizing quasi-spherical theory and Jahn-Teller distortion. This new material achieved high power density in piezoelectric energy harvesters.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Wan Ru Leow, Simon Voelker, Raoul Meys, Jianan Erick Huang, Shaffiq A. Jaffer, Andre Bardow, Edward H. Sargent
Summary: The production of hydrogen and hydrocarbon refining contribute significantly to CO2 emissions in the chemicals industry. Coupled electrification can cut emissions by up to 39%, even with the current electricity mix. Chemicals manufacturing is a major greenhouse gas emitter, with over half of the emissions coming from ammonia and oxygenates. By using electrolyzer systems that convert hydrocarbons to oxygenates and generate H-2 from water, emissions from fossil-based ammonia and oxygenates can be reduced by up to 88%. Low-carbon electricity is not necessary for a substantial reduction in global chemical industry emissions, as a 39% reduction can be achieved with the electricity carbon footprint available in the US or China today. Researchers interested in this area are provided with considerations and recommendations.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Richard Tran, Janice Lan, Muhammed Shuaibi, Brandon M. Wood, Siddharth Goyal, Abhishek Das, Javier Heras-Domingo, Adeesh Kolluru, Ammar Rizvi, Nima Shoghi, Anuroop Sriram, Felix Therrien, Jehad Abed, Oleksandr Voznyy, Edward H. Sargent, Zachary Ulissi, C. . Lawrence Zitnick
Summary: To address the lack of training data for oxide materials, researchers developed the OC22 dataset consisting of 62,331 DFT relaxations across various oxide materials. By combining the OC22 dataset with the OC20 dataset, significant improvements were achieved in energy predictions for oxide surfaces. This study provides an important benchmark for models aiming to incorporate complex electrostatic and magnetic interactions in oxide surfaces.
Article
Materials Science, Multidisciplinary
Ilgeum Lee, Omar Allam, Jiweon Kim, Yixuan Dou, Hyungju Ahn, Andrew Proppe, Yitong Dong, Dongxin Ma, Li Na Quan, Edward H. Sargent, Seung Soon Jang, Dong Ha Kim
Summary: Efficient blue-emitting materials with single-halide RPPs using organic spacer engineering are reported in this study. The (110)-oriented thin films exhibit larger bandgap and enhanced stability, regardless of the choice of spacers, compared to other structures. This new class of RPPs exhibits sky-blue emission at 483 nm with a quantum efficiency of approximately 62%. The established protocol and strategy can be utilized to develop blue perovskite LEDs.
ADVANCED OPTICAL MATERIALS
(2023)
Article
Chemistry, Physical
Jonathan P. Edwards, Theïo Alerte, Colin P. O'Brien, Christine M. Gabardo, Shijie Liu, Joshua Wicks, Adriana Gaona, Jehad Abed, Yurou Celine Xiao, Daniel Young, Armin Sedighian Rasouli, Amitava Sarkar, Shaffiq A. Jaffer, Heather L. MacLean, Edward H. Sargent, David Sinton
Summary: Carbon dioxide electrolysispowered with renewable electricity is a promising method for converting emissions into valuable chemicals and fuels. However, there are technological gaps that need to be addressed before industrial implementation, including pilot plant demonstrations and the development of accurate process models. In this study, a semi-empirical electrolyzer model was developed and validated using lab- and pilot-scale data. The results showed that the model can accurately predict the performance metrics of the electrolyzer, providing a foundation for further scaling of CO2 electrolysis.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Yujin Jung, Hyeyoung Shin, Se-Woong Baek, Truong Ba Tai, Benjamin Scheffel, Olivier Ouellette, Margherita Biondi, Sjoerd Hoogland, F. Pelayo Garcia de Arquer, Edward H. Sargent
Summary: Solution-processed semiconducting materials have potential for high-performance, low-cost, and flexible energy conversion devices. By using a library of surface ligands with different functions, the photophysical mismatch at the colloidal quantum dot (CQD)/organic interface was addressed, resulting in improved charge transfer efficiency. Hybrid CQD/organic heterojunction solar cells showed record photocurrent density and near-unity broadband quantum efficiency.
ACS ENERGY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Maria Caterina Giordano, Francesco Buatier de Mongeot, Debasree Chowdhury, Shaimaa A. Mohamed, Giacomo Manzato, Beatrice Siri, Roberto Chittofrati, Mohamed Hussein, Mohamed F. O. Hameed, Salah S. A. Obayya, Philipp Stadler, Markus C. Scharber, Giuseppe Della Valle
Summary: Thin-film organic photovoltaic (OPV) devices are being considered as a promising alternative to silicon solar cells due to their lightweight, flexibility, and low cost. However, the low optical absorption of OPV active layers is still a challenge. In this study, we demonstrate that nanostructured interfaces at the subwavelength scale, created through laser interference lithography and reactive ion etching, can significantly enhance the optical absorption in thin-film OPV devices. This large-scale light-harvesting strategy resulted in a 19% increase in optical absorption and a 14% increase in short-circuit current compared to flat devices, highlighting its potential in thin-film technologies.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Ping Fu, Michael A. Quintero, Eugenia S. Vasileiadou, Parth Raval, Claire Welton, Mikael Kepenekian, George Volonakis, Jacky Even, Yukun Liu, Christos Malliakas, Yi Yang, Craig Laing, Vinayak P. Dravid, G. N. Manjunatha Reddy, Can Li, Edward H. Sargent, Mercouri G. Kanatzidis
Summary: This study investigates two-dimensional alloyed Pb/Sn bromide perovskites in the Ruddlesden-Popper (RP) and Dion-Jacobson (DJ) phases using butylammonium and 3-(aminomethyl)pyridinium as spacer cations. The results show that the ratio and site preference of Pb/Sn atoms are influenced by layer thickness and spacer cations. Pb-rich alloys are thermodynamically favored in n = 1 compounds. Films in the RP phase exhibit parallel orientation to the substrate, while random orientations are observed for DJ cases.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
