Review
Chemistry, Applied
Jing Du, Yuan-Yuan Ma, Huaqiao Tan, Zhen-Hui Kang, Yangguang Li
Summary: Electrochemical CO2 reduction to value-added fuels and chemicals is an effective strategy due to its high efficiency and economic feasibility. Polyoxometalates (POMs) are promising candidates for efficient CO2RR electrocatalysts and play significant roles in the process and performance of catalytic CO2RR.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Kun Qi, Yang Zhang, Ji Li, Christophe Charmette, Michel Ramonda, Xiaoqiang Cui, Ying Wang, Yupeng Zhang, Huali Wu, Wensen Wang, Xiaolin Zhang, Damien Voiry
Summary: The study demonstrates a superstructure design using self-assembled two-dimensional silver nanoprisms to maximize the exposure of active edge ribs, resulting in enhanced selectivity and activity for the production of CO from CO2. The silver superstructures show high selectivity, current retention, and partial energy efficiency for CO production, with edge ribs identified as the active sites through electrochemical measurements.
Article
Chemistry, Physical
Ping Shao, Hai-Xia Zhang, Qin-Long Hong, Luocai Yi, Qiao-Hong Li, Jian Zhang
Summary: In this study, a tandem catalyst Ag@BIF-104NSs(Cu) was synthesized using ultrathin boron imidazolate framework (BIF) nanosheets as support to load Ag nanoparticles (Ag NPs). The highly ordered benzoate ligands decorated on the Cu sites of BIF-104NSs(Cu) allowed for atomic proximity of Ag NPs and Cu sites through coordination. Electrochemical CO2RR measurements demonstrated that this tandem catalyst significantly improved the selectivity and activity for CO2 reduction to ethylene. Density functional theory calculations revealed that the Ag sites in the composite efficiently reduce CO2 to *CO, which subsequently migrate to the Cu sites and form C2H4 through C-C coupling of the local enriched *CO.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Elisabeth Robens, Burkhard Hecker, Hans Kungl, Hermann Tempel, Ruediger-A. Eichel
Summary: The study demonstrates that the efficiency of electrochemical reduction of carbon dioxide to ethanol can be improved by synthesizing a bimetallic catalyst of silver and copper and decreasing the copper content. By reducing the near-surface copper content from 99% to 45%, the Faradaic efficiency of ethanol increases from 5% to 23%. Furthermore, the experiment also shows that the formation of ethanol is favored over ethylene by increasing the excess of CO, lowering the copper content, and increasing the silver near-surface content.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Xifeng Luo, Ran Jiang, Ziang Ma, Tiantian Yang, Hui Liu, Hui Deng, Wenhong Wu, Cunku Dong, Xi-Wen Du
Summary: This study elucidated the effect of Ag's work function on the electrochemical reduction of CO2 to CO by controlling the ratio of exposed crystalline planes. It was found that a higher proportion of Ag(110) to Ag(100) leads to a lower work function, resulting in enhanced electrochemical activity and selectivity for CO production. This research demonstrates a promising strategy to improve the electrochemical performance of metal catalysts by tuning their work functions through regulating exposed crystalline planes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Yitao Song, Yewang Peng, Shuang Yao, Peng Zhang, Yujie Wang, Jianmin Gu, Tongbu Lu, Zhiming Zhang
Summary: A simple and effective method for constructing highly efficient oxygen reduction catalysts with trace amount of isolated cobalt was developed by pyrolysis of Co-centered polyoxometalate@metal-organic framework (Co-POM@MOF). The resulting Co-W-NC composite catalysts exhibit excellent durability and high performance for oxygen reduction reactions.
CHINESE CHEMICAL LETTERS
(2022)
Article
Chemistry, Physical
Dominik Krisch, He Sun, Kevinjeorjios Pellumbi, Kirill Faust, Ulf-Peter Apfel, Wolfgang Schoefberger
Summary: This study reports the preparation and characterization of six easily assembled silver complexes and investigates the influence of ligand electronic properties on their performance in CO2 reduction. All the catalysts showed significant current enhancements in CO2-saturated solvents, without concurrent hydrogen evolution when using 2% H2O as a proton source. Preliminary studies demonstrated a promising Faradaic efficiency of 51% for CO at a current density of 50 mA cm(-2) when using a high-loading catalyst as an electrode in a flow cell with suitable electrolyte conditions.
Article
Chemistry, Physical
Libo Sun, Vikas Reddu, Tan Su, Xinqi Chen, Tian Wu, Wei Dai, Adrian C. Fisher, Xin Wang
Summary: Decorating carbon nanotubes with pyridine-based functional groups can enhance the activity of molecular catalysts towards CO2 reduction. Density functional theory calculations were conducted to support the experimental findings.
Article
Nanoscience & Nanotechnology
Li Zeng, Jun Shi, Hanxin Chen, Chong Lin
Summary: In this study, silver nanocubes were synthesized for the electrocatalytic reduction of CO2 to CO, showing excellent catalytic activity and long-term stability. This can be attributed to the stable low-index {111} facet of Ag nanocubes with low surface energy.
Article
Chemistry, Multidisciplinary
Nivedita Sikdar, Joao R. C. Junqueira, Denis Oehl, Stefan Dieckhoefer, Thomas Quast, Michael Braun, Harshitha B. Aiyappa, Sabine Seisel, Corina Andronescu, Wolfgang Schuhmann
Summary: Bimetallic tandem catalysts have emerged as a promising strategy for increasing the conversion rate of electrochemical CO2 reduction. A novel Cu/C-Ag nanostructured catalyst with an optimized Cu/Ag composition has been prepared, showing the highest CO2 conversion rate among the tested gas-diffusion electrodes.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Qiucheng Xu, Aoni Xu, Sahil Garg, Asger B. Moss, Ib Chorkendorff, Thomas Bligaard, Brian Seger
Summary: In this study, a descriptor called surface-accessible CO2 concentration ([CO2](SA)) was developed to indicate the limits of CO2-to-CO conversion in CO2 electrolysis. Three general strategies were identified to enrich [CO2](SA), resulting in improved performance. The maximum j(CO) achieved was 368 +/- 28 mA cm(geo)(-2) using a commercial silver catalyst.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Hua-Qing Yin, Lu-Lu Yang, Hao Sun, Hao Wang, Yu-Jie Wang, Min Zhang, Tong-Bu Lu, Zhi-Ming Zhang
Summary: W/Mo-doping electrocatalysts were developed using mixed-metal polyoxometalate as the precursor. Pt was transplanted on the surface of W/Mo@rGO via electroplating treatment to enhance the NRR performance. This study demonstrates the first highly efficient NRR electrocatalyst derived from mixed-metal polyoxometalate, showing outstanding stability and continuous catalytic performance.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Jiehao Du, Banggui Cheng, Huiqing Yuan, Yuan Tao, Ya Chen, Mei Ming, Zhiji Han, Richard Eisenberg
Summary: We report the unprecedented electrocatalytic activity of a series of molecular nickel thiolate complexes (1-5) in reducing CO2 to C1-3 hydrocarbons on carbon paper in pH-neutral aqueous solutions. Ni(mpo)(2) (3, mpo=2-mercaptopyridyl-N-oxide), Ni(pyS)(3)(-) (4, pyS=2-mercaptopyridine), and Ni(mp)(2)(-) (5, mp=2-mercaptophenolate) were found to generate C-3 products from CO2 for the first time in molecular complex. Compound 5 exhibits Faradaic efficiencies (FEs) of 10.6 %, 7.2 %, 8.2 % for C-1, C-2, C-3 hydrocarbons respectively at -1.0 V versus the reversible hydrogen electrode. Addition of CO to the system significantly promotes the FEC1-C3 to 41.1 %, suggesting that a key Ni-CO intermediate is associated with catalysis. A variety of spectroscopies have been performed to show that the structures of nickel complexes remain intact during CO2 reduction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Biotechnology & Applied Microbiology
Likun Luan, Xiuling Ji, Boxia Guo, Jinde Cai, Wanrong Dong, Yuhong Huang, Suojiang Zhang
Summary: Activation and conversion of CO2 into high-value-added products have become a promising approach to address environmental issues. This review comprehensively discusses the integration of enzymatic-electrocatalysis and microbial-electrocatalysis technologies for CO2 reduction, focusing on the electron transfer routes and the compatibility of electrode materials. The combination of solar energy-driven photo-electrochemical techniques with biocatalysis is also explored. The significant findings and future prospects of green and sustainable bioelectrocatalysis for CO2 reduction are highlighted, providing a blueprint for the production of valuable products from CO2 under efficient and mild conditions.
BIOTECHNOLOGY ADVANCES
(2023)
Review
Chemistry, Physical
Yating Zhu, Xiaoya Cui, Huiling Liu, Zhenguo Guo, Yanfeng Dang, Zhanxi Fan, Zhicheng Zhang, Wenping Hu
Summary: Electrochemical CO2 reduction through tandem catalysis has shown promise in enhancing efficiency, with limitations primarily due to high overpotential and poor selectivity in producing highly reduced carbon compounds. Recent advances in tandem catalysis for CO2RR have provided effective methods to improve performance, indicating potential for further research and development.
Article
Materials Science, Multidisciplinary
Tianqi Zhang, Renwu Zhou, Shuai Zhang, Rusen Zhou, Jia Ding, Fengwang Li, Jungmi Hong, Liguang Dou, Tao Shao, Anthony B. Murphy, Kostya (Ken) Ostrikov, Patrick J. Cullen
Summary: This study demonstrates successful ammonia synthesis from nitrogen and water using nonthermal plasma catalysis. The findings suggest that plasma-induced vibrational excitation and matched catalysts in the nonthermal plasma discharge reactor contribute to molecular dissociation. The results show that the ruthenium catalyst supported on magnesium oxide exhibits superior performance in ammonia production. This research highlights the potential of nonthermal plasma catalysis for sustainable ammonia production.
ENERGY & ENVIRONMENTAL 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
Chemistry, Multidisciplinary
Peng Zhou, Si-Xuan Guo, Linbo Li, Tadaharu Ueda, Yoshinori Nishiwaki, Liang Huang, Zehui Zhang, Jie Zhang
Summary: In this study, highly efficient carbon supported Ni-MoO2 heterostructured catalysts were reported for the electrochemical hydrogenation (ECH) of phenol in 0.10 M aqueous sulfuric acid (pH 0.7) at 60 degrees C. Catalysts with high and low densities of oxygen vacancy (O-v) sites achieved the highest yields of cyclohexanol and cyclohexanone, 95% and 86%, respectively, with faradaic efficiencies of approximately 50%. The enhanced phenol adsorption strength attributed to the O-v density was found to be responsible for the superior catalytic efficiency. This work provides a promising avenue for the rational design of advanced electrocatalysts for the upgrading of phenolic compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Ruoqi Chen, Hui Ma, Xinlei Ma, Tianhao Ai, Yuqiao Chai, Huanrong Zhang, Fengwang Li, Xusheng Wang, Chunhong Li, Junhui Ji, Mianqi Xue
Summary: Smart films, particularly smart Janus films based on thermoplastics, are essential components for smart devices. Traditional methods for preparing Janus films have limitations due to their high requirements and poor bonding forces. We developed a one-step solvent and antisolvent crystallization method to construct thermoplastics-based Janus films with excellent binding performance. By combining the optical and electrical properties of two-dimensional nanomaterials with the plasticity of thermoplastics, large-scale and low-cost intelligent thermoplastics can be created. Several proof-of-concept examples demonstrated the smart properties of these films, including plasticity, self-healing, reprocessibility, smart actuation, and recyclability, indicating a new direction for wearable devices.
CHEMICAL ENGINEERING JOURNAL
(2023)
Review
Chemistry, Multidisciplinary
Karolina Matuszek, Mega Kar, Jennifer M. Pringle, Douglas R. MacFarlane
Summary: Thermal energy storage technologies utilizing phase change materials can mitigate the intermittency issues of wind and solar energy by storing energy in the form of heat. However, the lack of practical phase change materials due to stability and safety concerns remains a major challenge.
Article
Chemistry, Multidisciplinary
Hoang-Long Du, Karolina Matuszek, Rebecca Y. Hodgetts, Khang Ngoc Dinh, Pavel V. Cherepanov, Jacinta M. Bakker, Douglas R. MacFarlane, Alexandr N. Simonov
Summary: Electrochemical lithium-mediated nitrogen reduction can be used to synthesize ammonia from renewables, but integrating it into electrolyzer devices is challenging due to the lack of understanding of the relationship between performance and proton transport parameters. In this study, a top-performance N-2 electroreduction system was used to investigate the correlation between reaction metrics and proton carrier properties, including alcohols, a phosphonium cation, tetrahydrofuran, a Bronsted acid, ammonium, and water. The study showed that optimized electrolyte compositions are required for productive carriers, and ammonia electrosynthesis with the phosphonium cation and iso-propanol achieved performance close to the ethanol benchmark. It was also found that ethanol undergoes irreversible degradation through reaction with oxidized solvent, unlike iso-propanol and phosphonium cation proton carriers.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Ying Zhang, Jianing Gui, Dan Wang, Junjun Mao, Chenchen Zhang, Fengwang Li
Summary: In this study, a tandem catalyst PDI-Cu/Cu with atomically isolated Cu-N sites and Cu clusters was synthesized, which showed more than 2 times the enhancement in C2H4 production compared with the non-tandem catalyst PDI/Cu. Density functional theory (DFT) calculations supported the tandem reaction mechanism, where Cu-N sites first reduced CO2 into highly concentrated CO and then CO migrated to the surfaces of Cu clusters for further conversion into C2H4, decoupling the complex C2H4 generation pathway at single active sites into a two-step tandem reaction. This work offers a rational approach to design electrocatalysts for boosting the selectivity of the CO2RR to C2+ products via a tandem route.
Article
Multidisciplinary Sciences
Yongxiang Liang, Jiankang Zhao, Yu Yang, Sung-Fu Hung, Jun Li, Shuzhen Zhang, Yong Zhao, An Zhang, Cheng Wang, Dominique Appadoo, Lei Zhang, Zhigang Geng, Fengwang Li, Jie Zeng
Summary: The authors report a coordination polymer catalyst with isolated neighboring copper sites that can efficiently reduce CO2 to C2H4 with high selectivity and stability under electrochemical conditions. This finding is significant for achieving net-zero carbon emissions through electrochemical CO2 reduction with renewable electricity.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Haoyue Sun, Rui Tang, Xingmo Zhang, Shuzhen Zhang, Wenjie Yang, Lizhuo Wang, Weibin Liang, Fengwang Li, Rongkun Zheng, Jun Huang
Summary: In order to address global warming and energy crisis, the development of photocatalysts with broad-range light-absorption and efficient carrier transfer is urgently needed for artificial photosynthesis and green chemical production. In this study, novel CsPbBr3 nanocrystal coupled NiFe-LDH (CPB/NiFe-LDH) Z-scheme photocatalysts were constructed for efficient photocatalytic CO2 reduction. The unique CPB/NiFe-LDH Z-scheme heterojunction allowed tailored photogenerated carrier transfer behaviors, resulting in significantly improved carrier transfer ability and reduction potential compared to pristine NiFe-LDH. By precisely controlling the CPB/NiFe-LDH ratio, tunable Z-scheme photocatalytic reduction capability and charge separation efficiency were achieved, with the optimal CPB/NiFe-LDH-2 photocatalyst showing a 2-fold increase in electron consumption rate compared to pristine NiFe-LDH. This work provides an innovative approach to construct photocatalysts with tunable Z-scheme charge transfer behavior, which can be applied in various solar energy conversion applications.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Physical
Tianlai Xia, Yu Yang, Qiang Song, Mingchuan Luo, Mianqi Xue, Kostya (Ken) Ostrikov, Yong Zhao, Fengwang Li
Summary: Recently, electrocatalytic reactions involving oxygen, nitrogen, water, and carbon dioxide have been developed to produce clean energy, fuels, and chemicals. Understanding catalyst structures, active sites, and reaction mechanisms is crucial for improving performance. In this review, we summarize state-of-the-art in situ characterisation techniques used in electrocatalysis, categorizing them into microscopy, spectroscopy, and other techniques. We discuss the capacities and limits of these techniques to guide further advances in the field.
NANOSCALE HORIZONS
(2023)
Review
Chemistry, Multidisciplinary
Peng Zhou, Jie Zhang
Summary: Replacing conventional fossil resources with renewable raw materials is crucial for achieving carbon neutrality and alleviating the energy crisis. Biomass, due to its natural abundance and ability to fix CO2, is considered a promising candidate for this purpose. Electrochemical conversion of biomass offers advantages such as operating at ambient conditions, scalability, and green generation of equivalents. This review discusses recent progress in electrochemical transformation of biomass, including catalysts, strategies for enhancing efficiency, and mechanistic understanding.
SCIENCE CHINA-CHEMISTRY
(2023)
Article
Chemistry, Physical
Madhurima Barman, Venkata Sai Sriram Mosali, Alan M. Bond, Jie Zhang, A. Sarkar
Summary: This study investigates the effects of morphology, specific surface area, and relative content of Cu/Cu-oxide in CuO-derived Cu electrocatalysts on the current density and product formation during electrochemical carbon dioxide reduction reaction (eCO(2)RR). The results show that the Cu-content of the CuO-derived Cu electrocatalysts determines the type of products and their corresponding faradic efficiencies, with higher initial Cu-content resulting in higher faradic efficiencies at lower negative potentials. Furthermore, it is found that high Cu-content, regardless of morphology, is particularly important for the formation of methane and formate. Therefore, this study reveals the relative roles of specific surface area and Cu/CuO-content of CuO-derived Cu electrocatalysts on the current densities, product formation, and associated faradic efficiencies in eCO(2)RR.
Article
Materials Science, Multidisciplinary
Thom R. Harris-Lee, Enrico Della Gaspera, Frank Marken, Jie Zhang, Cameron L. Bentley, Andrew L. Johnson
Summary: Aerosol-assisted chemical vapor deposition (AACVD) was used to fabricate highly nanostructured mixed anatase-rutile phase TiO2 using new and bespoke precursors. The precursor syntheses involved two steps and the suitability for AACVD was assessed using thermogravimetric analysis. The resulting TiO2 films showed exceptional OH- oxidation performance and promise for use in photoanodes for water splitting applications.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Physical
Douglas R. MacFarlane, Alexandr N. Simonov, Thi Mung Vu, Sam Johnston, Luis Miguel Azofra
Summary: The activation of dinitrogen plays a crucial role in the production of nitrogen compounds and is of fundamental importance in chemistry. This paper provides an overview of different approaches and their commonalities, aiming to establish connections for further advancements in sustainable nitrogen activation. Experimental aspects, including the positive role of increasing nitrogen pressure, are explored, along with insights on when N-15(2) experiments may or may not be necessary. Deconstructing the nitrogen reduction reaction, the paper offers a unified framework to understand the different approaches and components involved. Regarding sustainability, the authors argue that while green ammonia from a green-H-2-fed Haber-Bosch process seems promising, there is a pressing need for other sustainable approaches in real-world contexts.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Physical
Dale T. Duncan, Samantha L. Piper, Maria Forsyth, Douglas R. MacFarlane, Mega Kar
Summary: High-voltage sodium batteries are a promising solution for economical energy storage applications. Currently available electrolyte materials have limited success in such applications, thus the search for high-performing and safer alternatives is urgent. This study synthesizes six novel ionic liquids derived from two fluoroborate anions, which have shown great promise in recent battery literature. One of the synthesized ionic liquids, N-ethyl-N,N,N-tris(2-(2-methoxyethoxy)ethyl)ammonium (tetrakis)hexafluoroisopropoxy borate, exhibits promising physical properties and electrochemical performance, making it a potential high-voltage sodium electrolyte material.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)