Article
Chemistry, Physical
Martina Ruescher, Antonia Herzog, Janis Timoshenko, Hyo Sang Jeon, Wiebke Frandsen, Stefanie Kuehl, Beatriz Roldan Cuenya
Summary: Copper-based catalysts are widely used for the electrocatalytic CO2 reduction reaction (CO2RR) to convert CO2 into valuable industrial chemicals. Bimetallic materials, such as ZnO/Cu2O nanocubes, show promising catalytic performance for CO2RR. In this study, operando spectroscopy and data analysis were used to investigate the chemical and structural changes of the catalysts under CO2RR conditions. It was found that the addition of Zn affects the kinetics of subsurface processes, while the Cu surface layer remains unchanged. The presence of Zn stabilizes cationic Cu(i) species and increases the selectivity towards C2+ products, while Zn-rich alloy phases promote the formation of CO and the parasitic hydrogen evolution reaction.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Xianlong Zhou, Jieqiong Shan, Ling Chen, Bao Yu Xia, Tao Ling, Jingjing Duan, Yan Jiao, Yao Zheng, Shi-Zhang Qiao
Summary: This study proposes a solid solution strategy to stabilize Cu2+ ions by incorporating them into a CeO2 matrix, which improves the performance of Cu-based catalysts in CO2 reduction reaction and enhances the efficiency of CH4 production.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Pu Zhang, Xiaoyu Sui, Ying Wang, Zhuan Wang, Jiwu Zhao, Na Wen, Hailong Chen, Haowei Huang, Zizhong Zhang, Rusheng Yuan, Zhengxin Ding, Wenxin Dai, Xianzhi Fu, Yu-Xiang Weng, Jinlin Long
Summary: A series of novel surface Ru-H bipyridine complexes-grafted TiO2 nanohybrids were prepared for CO2 photocatalytic conversion to CH4 using H2 as electron and proton donors. The selectivity towards CH4 was significantly increased by ligand exchange with the surface Cp-RuH complex, resulting in a 4.4-fold enhancement in CO2 methanation activity. The optimal photocatalyst achieved an impressive CH4 production rate of 241.2 μL•g-1•h-1. Femtosecond transient IR absorption results showed the rapid injection of hot electrons into the conduction band of TiO2 nanoparticles, forming a charge-separated state responsible for CO2 methanation. The formation of CO2•- radicals through single electron reduction of CO2 molecules adsorbed on surface oxygen vacancies of TiO2 nanoparticles was identified as the critical step for the methanation, followed by insertion of radical intermediates into the explored Ru-H bond to generate Ru-OOCH species and ultimately CH4 and H2O in the presence of H2.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jinxia Liang, Hao Yu, Junjuan Shi, Bao Li, Lixin Wu, Ming Wang
Summary: In this paper, 2D monolayer and bilayer porphyrin-based metal-organic frameworks (MOFs) were successfully constructed by adjusting the reaction temperature and solvent polarity. The bilayer MOF showed 100% ultra-high selectivity for the reduction of CO2 to CO under simulated sunlight and could be recycled at least three times. The intrinsic mechanism of this photocatalytic CO2 reduction process was explored through experimental characterization and DFT calculations.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Wen-Dong Zhang, Yun Wang, Yi Liang, Ai-Lin Jiang, Hao Gong, Xiao-Ying Tian, Wen-Sheng Fu, Jia-Zhen Liao, Peng Chen, Ying-Zhao Ma
Summary: In this study, the Cu (I) MOF photocatalyst supported by 4'-(4-cynaophenyl)-4,2':6 & PRIME;,4-terpyridine was applied for the first time in the photocatalytic reduction of CO2. The micro-structural and physicochemical properties of the Cu (I) MOF were systematically studied, and it exhibited good performance and high selectivity in the reduction of CO2 to CO under full-spectrum and visible light illumination. The study demonstrates the potential of Cu (I) MOF as a photocatalyst with high selectivity and efficiency in CO2 reduction.
FRONTIERS IN CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Qin Chen, Weihao Mo, Guodong Yang, Shuxian Zhong, Hongjun Lin, Jianrong Chen, Song Bai
Summary: By developing a surface amorphization strategy, this study successfully fabricated crystalline@amorphous semi-core-shell cocatalysts, achieving a synergistic effect between crystalline core and amorphous shell, leading to enhanced efficiency and selectivity in the conversion of CO2 to chemical feedstocks.
Article
Nanoscience & Nanotechnology
Lei Jin, Ehab Shaaban, Scott Bamonte, Daniel Cintron, Seth Shuster, Lei Zhang, Gonghu Li, Jie He
Summary: Photocatalytic reduction of CO2 to valuable chemical fuels is of broad interest due to its potential to activate greenhouse gases using renewable energy input. The choice of metal cocatalysts and surface basicity of TiO2 can enhance the photocatalytic efficiency for CO2 photoreduction, with different metals showing varying activity and selectivity for CO and hydrocarbon production. The improvement of electron density and low proton affinity of metal cocatalysts play a key role in CO2 photoreduction.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Shaojie Wei, Qianqian Heng, Yufeng Wu, Wei Chen, Xiying Li, Wenfeng Shangguan
Summary: The research team successfully developed a novel Ag loaded mesoporous Ta2O5 photocatalyst with high selectivity and CO2 adsorption capacity using a SiO2 template method and in-situ photodeposition method, which can effectively promote the CO2 reduction reaction.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Organic
Pietro Franceschi, Elena Rossin, Giulio Goti, Angelo Scopano, Alberto Vega-Penaloza, Mirco Natali, Deepak Singh, Andrea Sartorel, Luca Dell'Amico
Summary: In this study, we developed a novel photocarboxylation method using an organic photoredox catalyst and different dihydropyridine compounds in combination with an organic base. Through mechanistic investigations, we discovered the key role of a hydrogen bonding complex between the dihydropyridine and the base. This method allowed for the synthesis of carboxylic acids under mild reaction conditions, with good yields and synthetic versatility.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Jingwen Jiang, Xiaofeng Wang, Qijun Xu, Zhiyuan Mei, Lingyan Duan, Hong Guo
Summary: A novel strategy for preparing highly selective and stable heterostructure photocatalysts with oxygen and nitrogen vacancies has been proposed, showing excellent photocatalytic reduction performances. The CO2 reduction mechanism has been confirmed and the results indicate potential applications in environmental catalysis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Jiaqi Feng, Limin Wu, Shoujie Liu, Liang Xu, Xinning Song, Libing Zhang, Qinggong Zhu, Xinchen Kang, Xiaofu Sun, Buxing Han
Summary: The influence of atomic dopants on the performance of Cu-based catalysts is investigated. Gd doping into Cu2O is found to effectively improve the catalyst's performance. The designed Gd1/CuOx catalyst exhibits excellent performance for CO2 electroreduction to C2+ products, due to its unique electronic structure and induced tensile strain.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Hao Li, Jianwu Sun
Summary: Gram-scale cubic silicon carbide nanoparticles with amorphous silicon oxide shell and abundant surface states are prepared through a simple mechanical milling approach, which enhances charge separation and prevents corrosion under visible light. The unique electronic properties of 3C-SiC nanoparticles address the challenge of low selectivity in photocatalytic CO2 reduction to C-1 compounds, achieving over 90% selectivity for CH4 production with efficient water oxidation.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Chengyang Feng, Tingting Bo, Partha Maity, Shouwei Zuo, Wei Zhou, Kuo-Wei Huang, Omar F. Mohammed, Huabin Zhang
Summary: This study demonstrates the enhancement of solar-driven CO2 reduction by modifying the surface coordination sphere. Decorating Mn atoms onto multi-edged TiO2 nano-pompons significantly improves CO2 adsorption and enables efficient charge transfer for reduction. The surface modulation strategy opens new avenues for photocatalytic CO2 reduction and rational design of highly efficient catalysts for clean energy conversion.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Hailing Huo, Fang Wu, Erjun Kan, Ang Li
Summary: The overall photocatalytic CO2 reduction reaction (PCRR) is crucial for CO2 utilization and solar energy conversion. However, efficient conversion remains a challenge. This Review summarizes strategies developed in the past decade, such as self-driving material development, Z-scheme heterojunction construction, cocatalyst loading, heteroatom doping, surface vacancy creation, and carrier-material matching. The future research directions in this field are also discussed.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Applied
Hengming Huang, Hui Song, Jiahui Kou, Chunhua Lu, Jinhua Ye
Summary: The photocatalytic conversion of CO2 into solar fuels is a promising approach for green and sustainable development, but challenges remain in achieving efficient CO2RR due to slow kinetics and unfavorable thermodynamics. Surface engineering strategies, such as introducing vacancies, dopants, and cocatalysts, can enhance the activity and selectivity of CO2RR by optimizing and regulating activation and reaction pathways through surface reconstruction. This review focuses on recent advances in the rational design of semiconductor surfaces for photocatalytic CO2RR, emphasizing improved CO2 adsorption, activation, and product selectivity through theoretical calculations and in situ characterization techniques. The goal is to provide a deep understanding and rational guidance for the design of semiconductors in photocatalytic CO2RR.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Ke Ye, Guiru Zhang, Xian-Yin Ma, Chengwei Deng, Xin Huang, Chonghao Yuan, Guang Meng, Wen-Bin Cai, Kun Jiang
Summary: The local reaction environment, especially the electrode-electrolyte interface near the cathode, plays a crucial role in defining the activity and selectivity of the electrochemical CO2 reduction reaction. A differential electrochemical mass spectroscopy approach on the Ag electrode was used to investigate this, leading to insights for optimized CO2-to-CO conversion performance. A multi-physics model with computational fluid dynamics and chemical simulation demonstrated the flow pattern and CO2 distribution, while spectroelectrochemical method investigated promotion effects on Ag catalyzed CO2 reduction.
ENERGY & ENVIRONMENTAL SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Qinglin Yuan, Jiajun Zhao, Dong Hyeon Mok, Zemin Zheng, Yixing Ye, Changhao Liang, Lin Zhou, Seoin Back, Kun Jiang
Summary: Se-based nanoalloys are a promising class of metal chalcogenides with tunable crystalline and electronic structures, showing great potential in renewable energy conversion and utilization. By controlling the alloying component, a flexible control over the oxygen reduction reaction pathway has been achieved, and an optimized scaling relationship between oxygenated ORR intermediates has been discovered on certain nanocrystals.
Article
Multidisciplinary Sciences
Jiajun Zhao, Cehuang Fu, Ke Ye, Zheng Liang, Fangling Jiang, Shuiyun Shen, Xiaoran Zhao, Lu Ma, Zulipiya Shadike, Xiaoming Wang, Junliang Zhang, Kun Jiang
Summary: Controlling the coordination environment of Pt can manipulate the 2e(-) or 4e(-) reduction pathways, leading to controlled product selectivity and H2O2 generation rate during oxygen reduction.
NATURE COMMUNICATIONS
(2022)
Article
Engineering, Multidisciplinary
Lei ZhiJie, Qian XiaoShi, Jiang Kun, Meng Guang
Summary: We have reported a highly band-selective, bifunctional meta-surface that can work as an ultra-wide perfect absorber for near-infrared (NIR) band as well as a visible-band sensor. The rational design strategy involves stacking and/or grating of metals, inorganic insulators, and stimuli-responsive materials. A PNIPAAm-based hydrogel layer was used as a stimuli-responsive insulator, which can reversibly swell and collapse in one dimension in response to stimuli, enabling the sensing capability in the visible band while maintaining perfect absorption in the NIR region.
SCIENCE CHINA-TECHNOLOGICAL SCIENCES
(2022)
Article
Chemistry, Analytical
Xian-Yin Ma, Wei-Yi Zhang, Ke Ye, Kun Jiang, Wen-Bin Cai
Summary: A balanced detection of both adsorbates and dissolved species is crucial for understanding the electrochemical reaction mechanism, but it remains challenging for different modes of electrochemical infrared spectroscopy. In this study, we report a novel electrochemical wide-frequency ATR-SEIRAS with a thin-layer flow cell design, enabling the simultaneous detection of surface and solution species.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Xiaojun Wang, Xuhao Wan, Xianxian Qin, Chi Chen, Xiaoshi Qian, Yuzheng Guo, Qunjie Xu, Wen-Bin Cai, Hui Yang, Kun Jiang
Summary: This study presents an electronic structure modulating strategy by dispersing RuO2 over defective TiO2 enriched with oxygen vacancies (RuO2/D-TiO2), which significantly enhances the acidic oxygen evolution reaction (OER) kinetics. The as-prepared RuO2/D-TiO2 catalyst exhibits good catalytic activity, low voltage, and long-term stability.
Article
Chemistry, Multidisciplinary
Jun Liu, Guiru Zhang, Ke Ye, Ke Xu, Yeliang Sheng, Can Yu, Hai Zhang, Qiaoxia Li, Zheng Liang, Kun Jiang
Summary: In this study, gram-scale carbon-supported single-atom catalysts were prepared using metallic and metalloid constituent-enriched gasification residual carbon via a top-down approach. The catalysts exhibited superior electrocatalytic performance for CO2-to-CO conversion in both H-type and membrane electrode assembly electrolyzers.
CHEMICAL COMMUNICATIONS
(2023)
Editorial Material
Chemistry, Multidisciplinary
Qiu Jiang, Kun Jiang, Yifan Ye, Kai Xi, Chuan Xia
FRONTIERS IN CHEMISTRY
(2023)
Article
Chemistry, Physical
Tian-Wen Jiang, Xianxian Qin, Ke Ye, Wei-Yi Zhang, Hong Li, Wenhui Liu, Shengjuan Huo, Xia-Guang Zhang, Kun Jiang, Wen-Bin Cai
Summary: This work addresses the key challenges in the electrochemical reduction of CO2 to formate (CO2RRTF) on Pd-based surfaces, including the identification of a high-performance catalyst and the validation of the reaction pathway. By studying the catalyst and mechanism interactively, a Bi-modified Pd/C catalyst is found to exhibit significantly improved activity, selectivity, durability, and extended working potentials for CO2RRTF. The mechanism of CO2 chemical hydrogenation on Pd surfaces is clarified, with monodentate formate identified as the key intermediate, through isotope labeled ATR-SEIRAS measurement, kinetic analysis, and DFT calculations.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Yicai Wu, Zijie Mao, Tian-Wen Jiang, Xian-Yin Ma, Li Zheng, Kun Jiang, Wen-Bin Cai
Summary: Polyethylene glycol (PEG) is commonly used as a suppressor for Cu interconnect electroplating in microelectronics manufacture, but its adsorption structure and its correlation with the inhibition effect have been unclear. This study utilizes ATR-SEIRAS spectroscopy to investigate the interfacial adsorption structure of PEG with Cl- on a Cu electrode, and provides evidence for the inhibition effect of PEG. The results show that the presence of Cl- causes a transformation in the conformation of PEG, favoring its adsorption on the Cu surface.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Dong Hyeon Mok, Hong Li, Guiru Zhang, Chaehyeon Lee, Kun Jiang, Seoin Back
Summary: By merging machine learning models and a selectivity map, we developed a high-throughput virtual screening strategy to predict the activity and selectivity of CO2RR catalysts, and discovered promising catalyst behaviors.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Guiru Zhang, Ke Ye, Baoxin Ni, Kun Jiang
Summary: This article reviews recent advances in using renewable electricity to convert CO2 into value-added chemicals and fuels. The focus is on the extrinsic reaction environment effects on CO2 conversion, and the assessment of prevailing hypotheses and experimental progress. The challenges and future opportunities for more efficient production of C2+ are also discussed.
Article
Chemistry, Multidisciplinary
Shuaiqi Gong, Baoxin Ni, Xiaoyang He, Jianying Wang, Kun Jiang, Deli Wu, Yulin Min, Hexing Li, Zuofeng Chen
Summary: Investigated the coordination of Cu single atoms on In2O3 to create a conceptual tandem photocatalyst. The catalyst achieves efficient CO2 reduction to C2+ products with simultaneous oxygen generation.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Electrochemistry
Ke Ye, Guiru Zhang, Baoxin Ni, Liang Guo, Chengwei Deng, Xiaodong Zhuang, Changying Zhao, Wen-Bin Cai, Kun Jiang
Summary: This study presents a differential electrochemical mass spectroscopic approach to investigate the complex environment of CO2 reduction reaction, which could contribute to the achievement of a sustainable circular carbon economy.