Article
Chemistry, Multidisciplinary
Shuai Yang, Xinyang Li, Jiawen Ma, Haiwei Guo, Yifeng Chen, Zhao Chen, Gengbo Ren, Xiaodong Ma
Summary: In this study, atomically dispersed Ru catalysts were synthesized and demonstrated to have good catalytic performance and stability for the oxidation of polychlorinated aromatic hydrocarbons.
Review
Chemistry, Physical
Sanshuang Gao, Tianran Wei, Jiaqiang Sun, Qian Liu, Dui Ma, Wenxian Liu, Shusheng Zhang, Jun Luo, Xijun Liu
Summary: Rechargeable aqueous Zn-CO2 batteries have great potential in addressing environmental problems and energy crises due to their utilization of CO2 and energy output. Developing efficient and stable CO2 reduction reaction (CO2RR) electrocatalysts is crucial for the advancement of this technology. Atomically dispersed metal-based catalysts (ADMCs), with high atom-utilization efficiency and superior catalytic activity, are being explored as promising candidates for Zn-CO2 batteries. Recent research has focused on the development of ADMCs, including transition metal and non-transition metal sites, and the relationship between active site structures and CO2RR activity/Zn-CO2 battery performance.
Article
Chemistry, Multidisciplinary
Libing Zhang, Jiaqi Feng, Shoujie Liu, Xingxing Tan, Limin Wu, Shunhan Jia, Liang Xu, Xiaodong Ma, Xinning Song, Jun Ma, Xiaofu Sun, Buxing Han
Summary: CO2 electroreduction plays a crucial role in reducing CO2 emissions and completing the carbon cycle. However, the formation of carbonates and low CO2 utilization efficiency in neutral or alkaline electrolytes hinder its commercial-scale application. In this study, a Ni-Cu dual atom catalyst supported on hollow nitrogen-doped carbon was designed for pH-universal CO2 electroreduction to CO. The catalyst exhibited a high CO Faradaic efficiency of approximately 99% in acidic, neutral, and alkaline electrolytes, with partial current densities of CO reaching 190 +/- 11, 225 +/- 10, and 489 +/- 14 mA cm(-2), respectively. Notably, the CO2 utilization efficiency under acidic conditions reached 64.3%, which was twice as high as that under alkaline conditions. The electronic interaction between Ni and Cu atoms was found to be responsible for the enhanced catalytic performance.
ADVANCED MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Xiangbin Cai, Xiaowen Chen, Zhehan Ying, Shi Wang, Yong Chen, Yuan Cai, Gen Long, Hongyang Liu, Ning Wang
Summary: ADCs have shown remarkable catalytic performance and can construct high-performance catalysts through strong metal support interactions. By controlling the coordination number of metals and introducing complementary species, the high tunability of metals can be achieved. In addition, nanodiamond@graphene support exhibits excellent thermal stability.
MATERIALS & DESIGN
(2021)
Article
Chemistry, Inorganic & Nuclear
Ruirui Yun, Beibei Zhang, Changsong Shi, Ruiming Xu, Junjie Mao, Zhaoxu Wang
Summary: In this study, atomically dispersed CuN3 catalysts supported by two different types of zirconia were fabricated to investigate the influence of the support on the electrocatalytic CO2 reduction towards CO. The CuN3/NC/T-ZrO2 catalyst exhibited excellent performance at a wide range of potentials, attributed to the acidic uncoordinated Zr4+ sites of T-ZrO2 and the conductivity enhancement of N-doped carbon (NC). Density functional theory calculations confirmed the effective decrease of Gibbs free energy for CO2 to CO conversion by T-ZrO2. Additionally, this study provided a promising strategy for tuning catalytic activity and selectivity by controlling the phase of the support, offering insights into the electrocatalytic CO2RR process.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Multidisciplinary
Jinxian Wang, Danni Deng, Qiumei Wu, Mengjie Liu, Yuchao Wang, Jiabi Jiang, Xinran Zheng, Huanran Zheng, Yu Bai, Yingbi Chen, Xiang Xiong, Yongpeng Lei
Summary: This review summarizes the recent progress of atomically dispersed (AD) copper catalysts as a chemically tunable platform for electrochemical CO2 reduction (ECO2R). It discusses the dynamic evolution, catalytic performance, and mechanism of these catalysts, as well as the prospects and challenges in the field. The review aims to contribute to the rational design of AD copper catalysts with enhanced performance for ECO2R.
Review
Chemistry, Inorganic & Nuclear
Zhun Zhang, Hengyu Li, Danfeng Wu, Lina Zhang, Jiwei Li, Junli Xu, Sen Lin, Abhaya K. Datye, Haifeng Xiong
Summary: This review focuses on the structure-performance relationship of atomically dispersed metal heterogeneous catalysts (ADHCs), specifically studying the influence of coordination environment on catalyst performance in both thermocatalysis and electrocatalysis. It provides insights into the future development of this field.
COORDINATION CHEMISTRY REVIEWS
(2022)
Review
Chemistry, Physical
Tao Gan, Dingsheng Wang
Summary: Catalysts can speed up chemical reaction rates and promote molecular transformation, which is significant in chemical industry and material science research. Atomically dispersed materials (ADMs) with highly active metal sites and fully utilized metal atoms have great potential in catalytic reactions. The adjustment of coordination environment and electronic structure allows for the construction of reactive centers with diverse properties.
Article
Chemistry, Multidisciplinary
Haoyang Ni, Zhenyao Wu, Xinyi Wu, Jacob G. Smith, Michael J. Zachman, Jian-min Zuo, Lili Ju, Guannan Zhang, Miaofang Chi
Summary: The atomic configurations of atomically dispersed catalysts (ADCs), such as atom-atom distances and clustering, greatly affect their catalytic performance. This study presents a CNN-based algorithm that can quantify the spatial arrangement of different adatom configurations. The algorithm was proven effective in accurately identifying atom positions and analyzing large data sets of ADCs. It offers a robust method to overcome the bottleneck in STEM analysis for ADC catalyst research and has the potential to be used as an on-the-fly analysis tool for catalysts in future in situ microscopy experiments.
Article
Chemistry, Multidisciplinary
Panpan Sun, Zelong Qiao, Shitao Wang, Danyang Li, Xuerui Liu, Qinghua Zhang, Lirong Zheng, Zhongbin Zhuang, Dapeng Cao
Summary: In order to achieve practical application of fuel cell, the development of highly efficient and durable Pt-free catalysts is crucial. In this study, atomically dispersed ZnNC catalysts with Zn-Pyrrolic-N-4 moieties and abundant mesoporous structure were prepared. The ZnNC-based anion-exchange membrane fuel cell (AEMFC) demonstrated ultrahigh peak power density and long-term stability, offering a new route for the advancement of AEMFCs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Yizhen Chen, Hanlei Sun, Bruce C. Gates
Summary: Metal nanoparticles on supports exhibit new catalytic properties when made smaller to the point of atomic dispersion. Advanced characterization techniques enhance understanding of catalyst performance, opening up possibilities for new discoveries in catalysis.
Review
Chemistry, Physical
Kuang Sheng, Guang Li, Jiayu Hao, Yanqiu Wang, Kaili Shi, Yang Liu, Ning Zhang, Xiaoqing Qiu, Min Liu, Wenzhang Li, Jie Li
Summary: This paper illustrates the relationship between the structure and multifunctional performance of mono-disperse catalysts using reversible oxygen electrocatalysis as an example. The progress in carbon-based and non-carbon-based mono-disperse catalysts is reviewed, and the prospects and challenges of mono-disperse catalysts for multifunctional electrocatalytic reactions are discussed.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Biophysics
Nannan Wu, Hong Zhong, Yu Zhang, Xiaoqian Wei, Lei Jiao, Zhichao Wu, Jiajia Huang, Hengjia Wang, Scott P. Beckman, Wenling Gu, Chengzhou Zhu
Summary: In this study, an atomically dispersed Ru3 site catalyst was used to catalyze small biomolecule oxidation, showing superior electrocatalytic ability compared to a Ru single-atom catalyst. The findings provide a new paradigm for designing promising catalysts to achieve highly sensitive and selective small biomolecule detection.
BIOSENSORS & BIOELECTRONICS
(2022)
Article
Multidisciplinary Sciences
Sang Eon Jun, Youn-Hye Kim, Jaehyun Kim, Woo Seok Cheon, Sungkyun Choi, Jinwook Yang, Hoonkee Park, Hyungsoo Lee, Sun Hwa Park, Ki Chang Kwon, Jooho Moon, Soo-Hyun Kim, Ho Won Jang
Summary: This study demonstrates the decoration of iridium single atoms (SAs) on silicon photoanodes, and assesses their role in separating and transferring photogenerated charge carriers. By embedding the iridium SAs in a NiO/Ni thin film, a benchmarking photoelectrochemical performance is achieved with high photocurrent density and stability. This research provides insights into the rational design of SAs on silicon photoelectrodes and the potential of iridium SAs in boosting photogenerated charge carrier kinetics.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Yunhu Han, Jun Dai, Ruirui Xu, Wenying Ai, Lirong Zheng, Yu Wang, Wensheng Yan, Wenxing Chen, Jun Luo, Qiang Liu, Dingsheng Wang, Yadong Li
Summary: The study presented a strategy to immobilize Ru atom using notched-polyoxometalate (N-POM) to prevent Ru aggregation during pyrolysis, leading to the successful synthesis of a Ru1@WOx/CN catalyst with outstanding catalytic activity for the hydrogenation of levulinic acid under solvent-free conditions. The N-POM strategy also shows potential in preparing a series of atomically dispersed noble-metal atoms, providing an opportunity for the discovery of single-atom catalysts.
Article
Chemistry, Multidisciplinary
Dong Cao, Zhirong Zhang, Yahui Cui, Runhao Zhang, Lipeng Zhang, Jie Zeng, Daojian Cheng
Summary: In this study, highly active catalysts consisting of high-density Pt and Ir single atoms anchored on Co(OH)(2) were constructed for green hydrogen production. The catalysts exhibited excellent catalytic activity and efficiency in alkaline water electrolysis, demonstrating great potential for practical applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Zhirong Zhang, Peiyu Ma, Lei Luo, Xilan Ding, Shiming Zhou, Jie Zeng
Summary: Regulating the spin state of active centers in transition metal oxides is of great significance in energy conversion processes. It directly modulates the metal-ligand bond strength and intermediate adsorption behavior. This review clarifies the importance of regulating the spin state and discusses characterization technologies and strategies to regulate the spin state. Lastly, future research directions in this field are proposed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Carlos E. Garcia-Vargas, Xavier Isidro Pereira-Hernandez, Dong Jiang, Ryan Alcala, Andrew T. DeLaRiva, Abhaya Datye, Yong Wang
Summary: We have successfully prepared a single atom Rh-1/CeO2 catalyst through the high temperature (800 degrees C) atom trapping (AT) method, which shows excellent stability under oxidative and reductive conditions. The presence of exclusively ionic Rh species was confirmed by infrared spectroscopy and electron microscopy characterization. The strong interaction between Rh and CeO2 achieved by the AT method ensures the stability of the ionic Rh species even under reducing conditions, resulting in high and reproducible CO oxidation activity. This is in contrast to catalysts synthesized by conventional impregnation approaches, where the ionic Rh species can be easily reduced to form Rh nanoclusters/nanoparticles and subsequently oxidized, leading to performance degradation.
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, Multidisciplinary
Lucas S. R. Cavalcante, Makena A. Dettmann, Tyler Sours, Dong Yang, Luke L. Daemen, Bruce C. Gates, Ambarish R. Kulkarni, Adam J. Moule
Summary: There is a need to develop new experimental and computational approaches to understand the structure and properties of defects in a wider variety of MOFs. In this study, low-frequency phonon modes measured by inelastic neutron scattering (INS) spectroscopy were combined with density functional theory (DFT) simulations to provide unprecedented insights into the defect structure of UiO-66. The INS/DFT approach provides detailed structural insights that are not accessible with microscopy-based techniques. Overall, this methodology may become part of the standard and preferred protocol for the characterization of MOFs.
MATERIALS HORIZONS
(2023)
Article
Environmental Sciences
Dong Hu, Jie Zeng, Jing Chen, Wenfang Lin, Xinyan Xiao, Mingbao Feng, Xin Yu
Summary: This study investigated the influence of roof tanks as an additional water storage device on the microbial community and pathogenic gene markers in urban villages. The results showed higher microbial concentrations in roof tank water samples compared to input water samples, especially in spring and summer. Pathogenic fungi and bacteria were frequently detected. Residual chlorine was identified as the driving force behind bacterial colonization and microbial community formation.
JOURNAL OF ENVIRONMENTAL SCIENCES
(2023)
Article
Chemistry, Multidisciplinary
Xiangdong Kong, Jiankang Zhao, Zifan Xu, Zhengya Wang, Yingying Wu, Yaohui Shi, Hongliang Li, Chuanxu Ma, Jie Zeng, Zhigang Geng
Summary: The structure of heterogeneous catalysts at the interface directly affects the reaction rate by controlling the adsorption behavior of reaction intermediates. In this study, a triazole-modified silver crystal (Ag crystal-triazole) with dynamic and reversible interface structures was developed to enhance the catalytic activity in the electroreduction of CO2 to CO. Through surface science measurements and theoretical calculations, the researchers demonstrated the dynamic transformation between adsorbed triazole and adsorbed triazolyl on the Ag(111) facet induced by metal-ligand conjugation. The dynamic metal-ligand coordination not only reduced the activation barriers but also altered the rate-determining step, leading to highly efficient CO2 electroreduction.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Chuanhao Wang, Junjie Du, Lin Zeng, Zhongling Li, Yizhou Dai, Xu Li, Zijun Peng, Wenlong Wu, Hongliang Li, Jie Zeng
Summary: The authors develop a universal strategy to synthesize extra-heavy olefins through the sustained release of hydrogen and selective extraction of olefins. They achieve the selective production of C(12+)(=) from CO and water using Pt/Mo2N and Ru particles as catalysts in polyethylene glycol (PEG). PEG acts as a selective extraction agent to hinder hydrogenation of olefins. Under optimal conditions, the yield ratio of CO2 to hydrocarbons reaches the theoretical minimum, and the C(12+)(=) yield reaches its maximum with a selectivity of 40.4%.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Jinshu Tian, Gregory Collinge, Simuck F. F. Yuk, Jindong Lin, Vassiliki-Alexandra Glezakou, Mal-Soon Lee, Yong Wang, Roger Rousseau
Summary: Through density functional theory calculations, in situ Raman characterization, and microkinetic modeling, it is found that dimerized di-coordinated boron sites are the active species for O-2 activation and peroxy-like structures are responsible for propane activation. The formation of adsorbed C3H7* radicals was found to be the main rate-controlling step. These findings provide significant insights into the mechanisms of oxidative dehydrogenation of propane on boron-based catalysts.
Article
Chemistry, Physical
Haibin Yin, Zhengtian Pu, Jiawei Xue, Peiyu Ma, Bo Wu, Mei Han, Hongfei Lin, Zhengtang Luo, Jie Zeng, Xinlong Ma, Hongliang Li
Summary: TiO2 nanorods with abundant oxygen vacancies enable the mild oxidation of methane by H2O2 into formaldehyde without light irradiation. The activity of TiO2 nanorods increases with the concentration of oxygen vacancies. The reaction intermediates and reaction scheme were identified based on catalytic and spectroscopic data.
Article
Chemistry, Physical
Yinyin Wang, Jiankang Zhao, Cong Cao, Jie Ding, Ruyang Wang, Jie Zeng, Jun Bao, Bin Liu
Summary: Selective electrochemical reduction of CO to acetate can be achieved on an amino functionalized Cu surface. The Cu@NH2 catalyst shows significant catalytic performance with a CO-to-acetate Faradaic efficiency of 51.5% and an acetate partial current density of around 150 mA cm-2 at -0.75 V versus RHE. The amino groups on the Cu surface help maintain the low valence state of Cu and the H delta+ in the amino groups stabilize the oxygen-containing intermediates, promoting the formation of acetate through *CO-*CHO coupling.
Article
Engineering, Environmental
Jinshu Tian, Jian Guan, Mingliang Xu, Shuya Qian, Kai Ma, Shaolong Wan, Zhaoxia Zhang, Haifeng Xiong, Shuai Wang, Yong Wang, Jingdong Lin
Summary: In this study, an efficient method for stabilizing hexagonal boron nitride (h-BN) with high specific surface area (SSA) under harsh conditions was proposed. The vacancy defects in h-BN were repaired with metal ions to significantly improve the antioxidant stability of the material. The repaired h-BN maintained a few-layer structure and exhibited high SSA and strong oxidation resistance, making it an excellent platform for fundamental studies and applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Gengrui Zhang, Yan Li, Yong Chen, Xinning Hao, Xianhua Zhang, Shuai Wang, Jingdong Lin, Yong Wang, Shaolong Wan
Summary: The study designs and prepares a nickel-based syngas methanation catalyst with superior thermal stability, using a special ZnAl2O4 spinel support. The catalyst shows excellent reactivity and stability. The work elucidates the critical role and intrinsic mechanism of the spinel support for the construction of the desired methanation catalysts.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Nanoscience & Nanotechnology
Junjie Du, Lin Zeng, Tao Yan, Chuanhao Wang, Menglin Wang, Lei Luo, Wenlong Wu, Zijun Peng, Hongliang Li, Jie Zeng
Summary: Ru nanoparticles on HZSM-5 catalyze solvent- and hydrogen-free upcycling of high-density polyethylene into separable linear (C-1 to C-6) and cyclic (C-7 to C-15) hydrocarbons. Plastic pollution, worsened by the COVID-19 pandemic, requires a sustainable and economically viable recycling method that avoids consumable materials. This study demonstrates the catalytic conversion of high-density polyethylene using Ru nanoparticles on HZSM-5, resulting in a separable distribution of linear and cyclic hydrocarbons.
NATURE NANOTECHNOLOGY
(2023)
Article
Multidisciplinary Sciences
Rui Zhang, Yong Wang, Pierre Gaspard, Norbert Kruse
Summary: In this study, the mechanistic steps underlying the formation of higher hydrocarbons in CO hydrogenation using cobalt-based catalysts at atmospheric pressure were investigated. The research revealed nonisothermal rate and selectivity oscillations that were sustained for extended periods of time. Experimental and theoretical analyses showed that temperature oscillations played a crucial role in the rate and selectivity oscillations, and the thermokinetic origin of these oscillations was supported by phase portraits.