Review
Chemistry, Physical
Kaiyuan Liu, Pengwan Chen, Zhiyi Sun, Wenxing Chen, Qiang Zhou, Xin Gao
Summary: Producing hydrogen peroxide (H2O2) through electrochemical oxygen reduction reaction (ORR) is a safe and green alternative to traditional anthraquinone processes. Single atom catalysts (SACs) have shown advantages in 2e(-) ORR catalytic production of H2O2, although their selectivity has been a challenge. This article reviews recent research on H2O2 production by SACs catalysis and emphasizes the importance of understanding the atomic interface of SACs in developing novel catalysts.
Article
Materials Science, Multidisciplinary
Mingwei Chang, Jing Wu, Li Xu, Liming Zhang
Summary: Renewable-energy-derived electrochemical nitrogen fixation is limited by sluggish kinetics and complex reaction pathways, thus requiring highly active, selective and robust electrocatalysts to enhance efficiency. This paper reviews the recent progress in understanding the structure-function correlation of single-atomic site catalysts (SASCs) for electrochemical nitrogen fixation and provides insights for future rational design. It covers the fundamental understanding of N-2 and oxynitride reduction on SASCs, the development of well-defined SASCs with various metal centres, and the influence from local chemical environments.
MATERIALS RESEARCH LETTERS
(2023)
Article
Chemistry, Physical
Seunghyuck Chi, Sang Gu Ji, Minho Kim, Hyungjun Kim, Chang Hyuck Choi, Minkee Choi
Summary: This study used in situ X-ray absorption spectroscopy to investigate the electrocatalytic properties of S-doped zeolite-templated carbon (SZTC) with 1-10 wt% Pt in the synthesis of H2O2. It was found that SZTC with a curved polyaromatic framework and abundant sulfur functional groups could stabilize isolated Pt sites. The specific activity of Pt increased rapidly with increasing Pt loading, and upon contact with aqueous electrolytes, only the labile sites were converted to true active sites via ligand exchange with water.
JOURNAL OF CATALYSIS
(2023)
Article
Engineering, Environmental
Zengxi Wei, Bowen Deng, Peng Chen, Teng Zhao, Shuangliang Zhao
Summary: In this study, several Pd-based single atom catalysts were designed, and it was found that C4Pd bound to defect graphene exhibited excellent activity and selectivity for H2O2 production. In contrast, Pd atomic clusters bound on defect graphene showed poorer performance.
CHEMICAL ENGINEERING JOURNAL
(2022)
Review
Chemistry, Physical
Qian Zhang, Lufan Zheng, Fangwei Gu, Jinting Wu, Jian Gao, Yong-Chao Zhang, Xiao-Dong Zhu
Summary: This article systematically describes the synthesis, characterization and catalytic mechanism of single-atom catalysts (SACs) for acidic oxygen reduction reactions (ORR) to produce hydrogen peroxide (H2O2). It highlights important activity descriptors, particularly the regulation methods for binding energy of oxygenated intermediates. The challenges and outlooks of using SACs for acidic ORR to H2O2 are also discussed.
Review
Chemistry, Multidisciplinary
Xiaoxuan Yang, Yachao Zeng, Wajdi Alnoush, Yang Hou, Drew Higgins, Gang Wu
Summary: Electrochemical oxygen reduction reaction (ORR) for generating hydrogen peroxide (H2O2) is a green alternative to traditional energy-intensive processes, and single metal site catalysts have emerged as promising ORR electrocatalysts. This article summarizes recent methodologies and achievements in developing these catalysts for selective reduction of O2 to H2O2. It also emphasizes the importance of catalyst stability and solutions to improve tolerance to H2O2, and highlights the challenges in translating catalyst properties to electrode performance for practical applications.
ADVANCED MATERIALS
(2022)
Article
Engineering, Environmental
Zhimin Gao, Qiuzi Zhu, Yanyan Cao, Cunshi Wang, Luming Liu, Jianzhong Zhu
Summary: This work presents elementary knowledge and theory of electrochemical H2O2 synthesis as well as the design strategies of carbon-based single-atom catalysts (SACs) for selective 2e(-) oxygen reduction reaction (ORR) H2O2 generation. It comprehensively reviews the selection of central metal atoms, modulation of coordinated atoms, and modification of environmental atoms for H2O2 selectivity production. Perspectives on the opportunities and challenges for selective electrochemical H2O2 production by carbon-based SACs are also provided based on understanding recent advances.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Chang Liu, Zixun Yu, Fangxin She, Jiaxiang Chen, Fangzhou Liu, Jiangtao Qu, Julie M. Cairney, Chongchong Wu, Kailong Liu, Weijie Yang, Huiling Zheng, Yuan Chen, Hao Li, Li Wei
Summary: By constructing heterogeneous molecular catalysts using cobalt porphyrins and carbon nanotubes, the catalytic properties and activity were successfully modulated, resulting in sustainable production of hydrogen peroxide with high selectivity and activity.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Shaoda Huang, Bingyan Zhang, Huimin Sun, Hongyin Hu, Jinyan Wang, Fang Duan, Han Zhu, Mingliang Du, Shuanglong Lu
Summary: We developed a series of single atom catalysts anchored on bipyridine-rich COFs. The optimal Py-Bpy-COF-Zn shows the highest selectivity of 99.1% and excellent stability in H2O2 production via oxygen reduction, attributed to its high *OOH dissociation barrier. As a proof of concept, it acts as a cathodic catalyst in a homemade Zn-air battery and enables efficient wastewater treatment.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Wenjun Zhang, Jae Won Choi, Sooyeon Kim, Thao Thi Le, Subhajit Nandy, Chang-Kyu Hwang, Sae Yane Paek, Ayeong Byeon, Keun Hwa Chae, Seung Yong Lee, Sang Hoon Kim, Hakhyeon Song, Jaehoon Kim, Jihun Oh, Jae W. Lee, Sang Soo Han, Jong Min Kim
Summary: By fine-tuning the coordination environment, a Co-N5-O-C catalyst with highly coordinated Co-N5 moieties and nearby electro-withdrawing epoxides was developed for efficient oxygen reduction reaction (ORR). This catalyst achieved optimal binding energy of *OOH intermediate, resulting in ultrahigh mass activity of 87.5 A g-1 and high H2O2 production rate of 11.3 mol g-1 h-1. It also enabled 100% degradation of organic methylene blue pollutant within 15 minutes through the electro-Fenton process, providing a new direction for on-site H2O2 synthesis and wastewater treatment.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Erhuan Zhang, Lei Tao, Jingkun An, Jiangwei Zhang, Lingzhe Meng, Xiaobo Zheng, Yu Wang, Nan Li, Shixuan Du, Jiatao Zhang, Dingsheng Wang, Yadong Li
Summary: Rarely reported is the in-depth understanding of local atomic environment-property relationships of p-block metal single-atom catalysts towards the 2e(-) oxygen reduction reaction (ORR). In this study, a heteroatom-modified In-based metal-organic framework-assisted approach is developed to synthesize an optimal catalyst, In SAs/NSBC, with accurately anchored single In atoms supported by hollow carbon rods. The catalyst exhibits a high H2O2 selectivity and unprecedented production rates in different electrolytes, providing practical guidance for H2O2 electrosynthesis and enabling the design of high-performance single-atom materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
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
Chemistry, Multidisciplinary
Jiarui Yang, Wen-Hao Li, Shengdong Tan, Kaini Xu, Yu Wang, Dingsheng Wang, Yadong Li
Summary: Catalysts designed by electronic metal-support interactions (EMSI), especially the single atomic site catalyst Rh1-TiC, show higher catalytic efficiency than Pt/C, with smaller overpotentials, lower Tafel slopes, and higher mass activities. Additionally, they demonstrate energy-saving advantages compared to Pt/C.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Bingyang Wang, Jin Lin, Qiangsheng Sun, Chungu Xia, Wei Sun
Summary: This study successfully developed bioinspired manganese catalysts using porous organic polymers (POPs) as scaffolds, which showed high reactivity in oxidation reactions and could be easily recycled and reused. The single-site nature of the catalyst prevented oxidative degradation during the reaction, making it a promising approach for selective oxidation reactions.
Review
Chemistry, Multidisciplinary
Jiexin Zhu, Lei Lv, Shahid Zaman, Xingbao Chen, Yuhang Dai, Shenghua Chen, Guanjie He, Dingsheng Wang, Liqiang Mai
Summary: This review summarizes the current research progress and future application prospects of electrochemical CO2 methanation on single-site catalysts (SSCs). It discusses the CO2 methanation mechanism, primary activity descriptors, coordination structure and design of SSCs, and several in situ characterization methods for tracking the structural changes in SSCs. This review provides insights into the further exploitation of SSCs for selective CO2 methanation and inspires the rational design of SSCs in electrochemical CO2 methanation research.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Shichao Ding, Jordan Alysia Barr, Zhaoyuan Lyu, Fangyu Zhang, Maoyu Wang, Peter Tieu, Xin Li, Mark H. Engelhard, Zhenxing Feng, Scott P. Beckman, Xiaoqing Pan, Jin-Cheng Li, Dan Du, Yuehe Lin
Summary: The introduction of phosphorus into Fe-N-C single-atom catalysts enhances the peroxidase-like activity, showing excellent selectivity and stability. A 1D carbon nanowire catalyst with enriched Fe-N-4 active sites and phosphorus doping is designed and synthesized, and it is employed in an enzyme cascade platform for highly sensitive colorimetric detection of the neurotransmitter acetylcholine.
ADVANCED MATERIALS
(2023)
Article
Agriculture, Multidisciplinary
Hongxin Xie, Xue Tian, Lina He, Jincheng Li, Liwei Cui, Xin Cong, Bochong Tang, Yi Zhang, Zhiying Guo, Aiyu Zhou, Dongliang Chen, Liming Wang, Jiating Zhao, Yong-Liang Yu, Bai Li, Yu-Feng Li
Summary: Spatial metallomics was used to visualize the distribution and speciation of selenium in a single seed of Cardamine violifolia in Enshi, China. The study found that methylated selenium species were mainly located in the seed coat, providing the first visual evidence of their in situ distribution in C. violifolia seeds. This research deepens our understanding of selenium tolerance in C. violifolia and could have implications for studying tolerance of heavy metals/metalloids in other hyperaccumulators.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2023)
Article
Chemistry, Physical
Liye Zhu, Hong Zhong, Dan Du, Tao Li, Hoai Nguyen, Scott P. Beckman, Wentao Xu, Jin-Cheng Li, Nan Cheng, Yuehe Lin
Summary: Single-atom catalysts have attracted attention in cancer therapy due to their high catalytic activity and stability. In this study, Fe-N-5/GN SAC was designed and synthesized, which exhibited exceptional peroxidase-like catalytic activity and could kill lung cancer cells by decomposing H2O2 under an acidic microenvironment.
Review
Chemistry, Analytical
Fengyang Zhao, Wenli Wu, Mei Zhao, Shichao Ding, Yuehe Lin, Qiongzheng Hu, Li Yu
Summary: This paper reviews the recent progress of enzyme-like materials integrated microfluidic platforms for various bioanalysis. The types of enzyme-like nanomaterials and various applications are summarized. In the end, the current challenge and perspective are also discussed.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Hao Hu, Yu Meng, Yi Mei, Peng-Xiang Hou, Chang Liu, Hui-Ming Cheng, Minhua Shao, Jin-Cheng Li
Summary: A bifunctional oxygen electrocatalyst enriched with single Fe atoms and NiFe2O4 nanoparticles is designed to enhance the performance of rechargeable zinc-air batteries. It accelerates the oxygen reduction reaction during discharging and promotes the oxygen evolution reaction during charging. The catalyst demonstrates excellent durability and enables high power density and low voltage loss for the corresponding zinc-air battery.
ENERGY STORAGE MATERIALS
(2023)
Review
Chemistry, Analytical
Linlin Wang, Wenlei Zhu, Jianrong Zhang, Jun-Jie Zhu
Summary: Electrochemical biosensors, utilizing enzymatic biofuel cells as energy and signal generators, have become a research hotspot due to their power self-support and simplified structure. Enzymatic biofuel cell-powered biosensors (EBFC-SPBs) have achieved tremendous success in health monitoring, but the miniaturization of portable EBFC-SPBs remains challenging. Microfluidic technology has significantly contributed to the progress of miniaturized and portable EBFC-SPBs. This review summarizes the achievements and progress in miniaturized EBFC-SPBs and discusses the advantages and challenges of microfluidic and screen-printing technologies for wearable and disposable EBFC-SPBs.
Article
Chemistry, Multidisciplinary
Ju-Zhen Zhang, Zichu Zhang, Hong-Bo Zhang, Yi Mei, Feng Zhang, Peng-Xiang Hou, Chang Liu, Hui-Ming Cheng, Jin-Cheng Li
Summary: A method based on Prussian-Blue analogue was proposed to prepare honeycomb-like ultrathin and heterogeneous Co2P-Fe2P nanosheets. These nanosheets exhibited low overpotentials for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline, acidic, and neutral electrolytes. The nanosheets also showed excellent performance in universal-pH water electrolysis, achieving high efficiency at ultralow voltages under alkaline conditions.
Article
Biochemistry & Molecular Biology
Chuanrui Chen, Shichao Ding, Joseph Wang
Summary: Growing life expectancy presents challenges for strained health systems. Digital technologies have the potential to transform geriatric care and enable remote monitoring, promoting health and independence in aging populations. This Perspective summarizes the progress, challenges, and future opportunities of digital technologies in geriatric care, with a focus on wearables for health monitoring and maintaining independence at home.
Review
Chemistry, Analytical
Minling Ding, Shichao Ding, Dan Du, Xin Wang, Xiaoling Hu, Ping Guan, Zhaoyuan Lyu, Yuehe Lin
Summary: Alzheimer's disease is a progressive neurodegenerative disorder with a long latency. Accurate diagnosis and early treatment are crucial for better therapeutic outcomes. Detection of body fluid biomarkers, particularly amyloid beta(1-42), is an effective strategy for early diagnosis. Electrochemical biosensors offer advantages in monitoring amyloid beta(1-42) levels due to their speed, portability, and on-site analysis capabilities.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Review
Chemistry, Analytical
Zhaoyuan Lyu, Jiachi Zhou, Shichao Ding, Dan Du, Joseph Wang, Yun Liu, Yuehe Lin
Summary: Single-atom catalysts and nanozymes have gained significant attention in the field of catalysis. Compared to natural enzymes, nanozymes exhibit stronger catalytic activity and higher cost-effectiveness. This review comprehensively overviews the applications of nanozymes in colorimetric biosensing and discusses strategies to improve their catalytic efficiency.
TRAC-TRENDS IN ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Ponnusamy Nandhakumar, Cristina Munoz San Martin, Beatriz Arevalo, Shichao Ding, Mahika Lunker, Eva Vargas, Omeed Djassemi, Susana Campuzano, Joseph Wang
Summary: In order to address the low sensitivity issue of conventional LFA, we report a simple electrochemical LFA with nanocatalytic redox cycling for decentralized insulin detection. This method achieves higher sensitivity than traditional methods by amplifying the signal through nanoparticles and chemical reactions.
Article
Multidisciplinary Sciences
Ye Ye, Zhe Li, Shichao Ding, Jiaju Fu, Hongzhi Liu, Wenlei Zhu
Summary: This paper investigates the recent progress of electrocatalytic C-N coupling reactions and explores the potential of coupling CO2 reduction with nitrogen (N)-pollutants reduction. The technical concerns for scale-up applications of C-N coupling electrocatalysis are discussed, and the opportunities and challenges of applying C-N coupling electrocatalysis are prospectively analyzed.
Article
Chemistry, Multidisciplinary
Juan Liu, Xiaoxiao Guo, Zhaoyuan Lyu, Rong-Bin Song, Pengyu Zhou, Shichao Ding, Yang Zhou, Li-Ping Jiang, Yuehe Lin, Wenlei Zhu
Summary: By using copper electrocatalysts and microorganisms, an electro-bio tandem reactor was designed to convert CO2 into specific multicarbon compounds in both the gas and liquid phases. The reducing products from electrocatalysis can be consumed and recycled for selective acetate synthesis in Moorella thermoacetica. The results showed high faradaic selectivity for acetate in liquid products for Cu-based CO2 electroreduction and high electron conversion rate to ethylene and acetate for microbial electrosynthesis, presenting a green design for CO2 upcycling targeting multicarbon products through the parallel integration of electrocatalysis and fermentation.
Review
Energy & Fuels
Su Hui, Yujing Jiang, Yuanfan Jiang, Zhaoyuan Lyu, Shichao Ding, Bing Song, Wenlei Zhu, Jun-Jie Zhu
Summary: This paper systematically summarizes recent advancements in cathode materials in the field of electrocatalyst-assisted and photocatalyst-assisted microbial electrosynthesis (MES). Various material types are compared to investigate their effects on production rate and conversion efficiency. The paper also discusses the prospects for future development and practical applications of MES, providing theoretical guidance for the fabrication of cathode materials.
