Article
Engineering, Multidisciplinary
Behnam Seyyedi, Bafrin Shakhseh
Summary: This study introduces a Cobalt-rGO composite with excellent activity for converting oxygen to hydrogen peroxide and producing electrochemical energy. The composite exhibits good catalytic performance, economical synthesis method, high specific surface area, high selectivity, and electrochemical durability.
ALEXANDRIA ENGINEERING JOURNAL
(2022)
Article
Energy & Fuels
Jing Zhang, Junyu Yang, Yan Wang, Haiqiang Lu, Mingang Zhang
Summary: Two types of CoN4-graphene catalysts were studied, with CoN4-G(A) showing higher catalytic activity and CoN4-G(B) showing higher 4-electrons selectivity. Both models exhibited ORR activity, with CoN4-G(A) allowing 2-electrons and 4-electrons pathways, while CoN4-G(B) favoring only the 4-electrons ORR pathway.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2021)
Article
Chemistry, Physical
Cehuang Fu, Liuxuan Luo, Lijun Yang, Shuiyun Shen, Xiaohui Yan, Jiewei Yin, Guanghua Wei, Junliang Zhang
Summary: The study systematically investigates the influence of non-metal elements doping (B, N, Si, P, S) on the ORR catalytic activity of Co-gN(4) based on density functional theory. It is found that different doping elements have different effects on the ORR process, with P and S doping showing a promotion effect on the ORR activity.
Article
Chemistry, Physical
Qingming Deng, Jin Han, Jiong Zhao, Guibin Chen, Tejs Vegge, Heine Anton Hansen
Summary: In this study, we investigate the stability and reaction mechanisms of synthesized one-dimensional transition metal dithiolene wires for the oxygen reduction reaction and the oxygen evolution reaction in acid solution using density functional theory calculations. Our results show that CoDW exhibits high catalytic activity for bi-functional ORR/OER with low limiting overpotentials through four-electron reactions, and by applying uni-axial strain, the adsorption strength of reaction intermediates on transition metal reactive sites can be optimized. These findings provide valuable insights into the rational design of non-precious metal-based electrocatalysts and suggest a new strategy of tuning adsorptions via uni-axial strain to develop efficient bifunctional electrocatalysts for ORR/OER.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Tiantian Fu, Guijun Li, Yang Xiang, Yibo Tang, Dongping Cai, Shuangshi Jiang, Yu Xue, Zhongping Xiong, Yujun Si, Chaozhong Guo
Summary: The synthesized bifunctional oxygen electrocatalyst Co-UA-OCB with heavy nitrogen content exhibits remarkable activity for oxygen reduction and evolution reactions, showing promising potential for rechargeable Zn-air batteries.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Chemistry, Physical
Ningning Wang, Xiaoguang Zheng, Yaer Buba, Hairui Wang, Xiaojing Wang, Yanhong Zhao
Summary: Electrocatalysts based on nanosized cobalt or nickel particles encapsulated by nitrogen-doped carbon nanotubes (M@NCNTs (M = Co or Ni)) were synthesized and showed excellent catalytic activity towards oxygen reduction reaction (ORR) in an alkaline electrolyte. The Co@NCNT catalyst had a higher half-wave potential (E1/2) of 0.881 V compared to commercial Pt/C (0.856 V), and both Co@NCNT and Ni@NCNT catalysts exhibited good stability in ORR. Density functional theory calculations revealed strong OOH absorption on the C atoms adjacent to pyridinic N in the Co@NCNT and Ni@NCNT catalysts.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Meena Rittiruam, Siriwimol Somdee, Puwit Buapin, Nuttanon Aumnongpho, Nuttapat Kerdprasit, Tinnakorn Saelee, Soorathep Kheawhom, Nutchapon Chotigkrai, Supareak Praserthdam, Piyasan Praserthdam
Summary: The study investigates the deactivation mechanisms of alpha-manganese dioxide electrocatalyst during charge-discharge cycling using density functional theory-based analysis, attributing the deactivation to phase transformation from alpha-MnO2 to beta-MnO2 and the formation of the limiting *OOH species during oxygen reduction reaction. It suggests that preventing phase transformation is crucial for high-performance MnO2-based electrocatalysts for ORR/OER.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Engineering, Environmental
Jinlong Liu, Juanxiu Xiao, Bingcheng Luo, Enke Tian, Geoffrey I. N. Waterhouse
Summary: By using density functional theory calculations, it was found that the central metal and coordinating atoms strongly influence the oxygen electrocatalysis activity on metal single-atom catalysts, primarily by tuning the adsorption free energy of adsorbed hydroxyl. Dual limiting potential volcano curves were constructed, with Ni-N2-C identified as the optimal synthetic target for bifunctional ORR/OER electrocatalysis.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Applied
Zhongjing Deng, Xingqun Zheng, Mingming Deng, Li Li, Li Jing, Zidong Wei
Summary: The research investigates the potential of TM single atoms supported by V2CO2 in two-dimensional materials for ORR and HOR catalysis, finding that Mn- and Sc-V2CO2 exhibit high catalytic activity and stability, serving as excellent bifunctional catalysts for fuel cells.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Dong Yun Shin, Yeon-Jeong Shin, Min-Su Kim, Jeong An Kwon, Dong-Hee Lim
Summary: In this study, Pt-based binary alloys were investigated for oxygen reduction reaction, and it was found that the addition of a single Pt skin layer on top of Pt-M alloys can enhance ORR performance by decreasing the adsorption strengths of key intermediates. This approach offers the benefit of decreased Pt content while maintaining high performance in fuel cell catalysts.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Xiaoqin Feng, Zeying Xu, Jiong Zhao, Heine Anton Hansen, Qingming Deng
Summary: This study systematically explores the potential of synthesized one-dimensional transition metal salen-type complexes (TM-SCs) as bi-functional electrocatalysts for ORR and OER through computational screening. Different macrocyclic ligands play a crucial role in governing the catalytic performances, with Co-SCs showing the highest bifunctional catalytic activities. The excellent electrocatalytic performance of Co salen-based chain is highlighted, showing promising implications for catalyst optimizations.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Energy & Fuels
Ji-Woo Park, Young-Wan Ju
Summary: Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial for energy systems like fuel cells and metal-air batteries. Precious metal catalysts, such as Pt and IrO2, have been widely used but their drawbacks necessitate the development of alternative electrochemical catalysts. Transition metal oxides, including Co3O4 and CoFe2O4, show similar ORR and OER activities to precious metal catalysts, making them potential alternatives. In this study, composite catalyst materials were synthesized using hydrothermal synthesis, and they exhibit bi-functional electrochemical catalytic activity for ORR and OER due to their unique nanostructure.
Article
Materials Science, Multidisciplinary
Qian Liu, Bin Yu, Xiaobin Liao, Yan Zhao
Summary: The mechanisms and activities of oxygen reduction reaction (ORR) on the (110) and (111) surfaces of Co3O4 were investigated using density functional theory (DFT) calculations. It was found that the (110) type B surface exhibited better ORR activity, with the rate-determining step depending on *OH desorption. Considering solvent effects, chemically adsorbed water molecules enhanced the ORR activity. The most favorable ORR pathway was determined to be O-2 -> *O-2 -> *OOH -> *O + H2O -> *OH -> H2O.
ENERGY & ENVIRONMENTAL MATERIALS
(2021)
Article
Engineering, Environmental
Xin Chen, Haiye Zhu, Junqing Zhu, Hui Zhang
Summary: This study investigates the catalytic performance of indium-based bimetallic clusters anchored onto silicon-doped graphene as multifunctional electrocatalysts. It identifies In2V2/Si-G and In2Co(2)/Si-G as potential trifunctional (ORR/OER/HER) electrocatalysts with low overpotentials.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Tipaporn Patniboon, Heine Anton Hansen
Summary: This study systematically investigated the catalytic activity and stability of metal-nitrogen carbon catalysts in acidic conditions using density functional theory, identifying acid-stable and active MNx structures for oxygen reduction reaction. The findings provide helpful guidance for the rational modification of carbon matrices hosting MNx moieties and the selection of metal atoms to optimize activity and stability in the ORR.
Article
Chemistry, Physical
Xin Chen, Yizhen Zhang, Shangyu Lin, Hui Zhang, Xiuyun Zhao
Summary: In this work, the activity of transition metal substituted Mo2CTx for oxygen reduction reaction (ORR) is investigated. It is found that TM-Mo2CTx has the potential for catalyzing ORR after the substitution of TM. Three TM-Mo2CTx catalysts, Mn-, Fe-, and Ni-Mo2CTx, exhibit ultrahigh ORR activity and outperform Pt(111) and other reported ORR catalysts. The origin of the ultrahigh ORR activity of Mn-Mo2CTx is revealed by analyzing the electronic structure. This study demonstrates that incorporating transition metals into Mo2CTx lattice is an effective strategy to enhance its ORR performance and provides guidance for the design of this novel MXene electrocatalyst.
SURFACES AND INTERFACES
(2023)
Article
Energy & Fuels
Lincheng Xu, Yue Wang, Yong Yan, Zhanzhong Hao, Xin Chen, Fan Li
Summary: Understanding the rare-earth mediated modulation of electronic structure and orbital filling in perovskites is crucial for designing highly active catalysts. This study doped LaMnO3 with Gd3+ at the A-site, triggering the B-site active center and improving the covalency of Mn-O bond and oxygen vacancy concentration. DFT calculations revealed optimized electronic structure and catalytic activity in La0.8Gd0.2MnO3, resulting in improved performance of zinc-air cells with La0.8Gd0.2MnO3 as the cathode catalyst.
Article
Chemistry, Physical
Xin Chen, Yu Dai, Hui Zhang, Xiuyun Zhao
Summary: In this paper, the catalytic performance of picket fence cobalt porphyrin and its atropisomer for oxygen reduction reaction (ORR) are investigated by density functional theory methods. According to the structural characteristics, they are named alpha alpha alpha alpha and alpha beta alpha beta, respectively, and three catalytic sites are considered for them. The *O-2 is adequately activated on all studied sites, which is favorable for the further progress of ORR. For alpha alpha alpha alpha-I and alpha alpha alpha alpha-II, *OOH is more easily hydrogenated to form *O + H2O, showing better selectivity for 4e(-) ORR. In contrast, alpha beta alpha beta tends to catalyze ORR through the 2e(-) pathway.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2023)
Article
Engineering, Chemical
Detang Guo, Jiangshan Liu, Xiuyun Zhao, Xu Yang, Xin Chen
Summary: Density functional theory calculations were performed to investigate CO2 adsorption and initial conversion on Pd12M (M = Fe, Co, Ni, Cu, Zn, Ru, Rh, Pd, Ag, Cd) bimetallic clusters, with a focus on identifying the optimal ancillary metal to Pd. The stability analysis showed that the doped Pd13 clusters with transition metals having higher surface energy than Pd exhibited better structural stability. The structural parameters of CO2* were found to have a significant linear relationship with the amount of charge transfer.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Engineering, Chemical
Xin Chen, Liang Luo, Shihong Huang, Xingbo Ge, Xiuyun Zhao
Summary: Recently, metal-organic frameworks have been widely studied for their potential as catalytic materials in electrocatalytic applications. This study focuses on investigating the catalytic activities of heterometallic cluster-based organic frameworks in the oxygen reduction reaction and oxygen evolution reaction. The results show that Fe2Mn-Mn exhibits the lowest overpotential for the oxygen reduction reaction, and Fe2Co-Co exhibits the lowest overpotential for the oxygen evolution reaction, surpassing the catalytic activities of conventional catalysts. Furthermore, the mixed-metal cluster strategy is found to enhance the electronic properties and catalytic activity of the catalyst. Overall, this study demonstrates the potential of mixed-metal clusters as high-efficiency bifunctional electrocatalysts.
FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING
(2023)
Article
Chemistry, Physical
Qin Chen, Qiang Ke, Xiuyun Zhao, Xin Chen
Summary: The electronic properties of catalyst surfaces can be modified by doping with foreign metals, leading to changes in catalytic activity. In this study, first-principles calculations were used to investigate how indium doping affects the catalytic activity of stepped Rh(211) for methanol synthesis. The results showed that indium atoms preferentially dope at the step edge of Rh(211). Adsorption of species was found to occur mainly at the step-edge sites due to the lowest coordination number of surface atoms at the step edge. The activation degree of CO2* was found to depend on the charge transfer between CO2* and the catalyst. The presence of indium atoms increased the number of H* adsorption sites on In/Rh(211) and promoted the relative stability of adsorbed species. Additionally, indium doping significantly inhibited the generation of by-product CO*, resulting in a low activation barrier for the rate-determining step on In/Rh(211). The ultrahigh catalytic activity of In/Rh(211) could be attributed to the decreased work function induced by indium doping, enhancing the relative stability of reaction species and the activation degree of CO2*.
MOLECULAR CATALYSIS
(2023)
Article
Chemistry, Physical
Xin Chen, Yahui Li, Xiuyun Zhao
Summary: Designing efficient electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is crucial for energy storage, conversion, and sustainable development. This study investigates the replacement of Ni atoms in two-dimensional MOF materials (Ni-2D-SA and Ni-O-2D-SA) with 3d, 4d, and 5d transition metals to screen for electrocatalysts with high bifunctional activity and stability for ORR and OER. The results suggest that Ir-2D-SA and Co-O-2D-SA are the most promising bifunctional electrocatalysts based on their low overpotentials and potential gap values. This work provides theoretical guidance for the development of efficient ORR and OER electrocatalysts.
SURFACES AND INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Xiaotao Liang, Qiang Ke, Xiuyun Zhao, Xin Chen
Summary: The impact of adjusting the N coordination number in Sn single-atom catalysts on the activity and selectivity of CO2 hydrogenation to HCOOH is investigated. Density functional theory calculations determine that Sn-NxC4-x-G (x = 1-4) catalysts are structurally stable. The reaction mechanism reveals that the optimal path for CO2 hydrogenation to HCOOH involves CO2* + H2* -> HCOO* + H* -> HCOOH*. The catalytic activity order of Sn-NxC4-x-G is determined to be Sn-N1C3-G > Sn-N2C2-G > Sn-N3C1-G > Sn-N4-G. The p-band center of the Sn atom is a good descriptor for evaluating the catalytic activity for HCOOH synthesis in the Sn-NxC4-x-G system.
ACS APPLIED NANO MATERIALS
(2023)
Article
Engineering, Environmental
Yahui Li, Yingjie Feng, Desheng Zheng, Xiuyun Zhao, Yue Zhou, Xiaoyue Fu, Xin Chen
Summary: In this study, the bifunctional catalytic activity of transition metal-doped carbon-nitride materials was investigated for the oxygen electrode reaction in metal-air batteries. The results show that certain transition metal-doped carbon-nitride materials exhibit comparable or even better catalytic activity than traditional catalysts, offering potential for improving the performance of metal-air batteries.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Liu Jing, Gao Jie, Wanqing Yu, Huanwei Ren, Xuejing Cui, Xin Chen, Luhua Jiang
Summary: In this study, a highly active and stable electrocatalyst Ru-TiO/TiO2@NC is developed for hydrogen oxidation and evolution reactions. The catalyst exhibits exceptional activity and stability, outperforming the traditional Pt/C catalyst. The unique sandwich structure and optimized interaction between Ru and TiO/TiO2 contribute to the enhanced performance of this Ru-based catalyst.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Chengyi Lu, Yuchen Wu, Yi Rong, Haiye Zhu, Xin Chen, Tianyi Gu, Zhengyi Lu, Mark H. Rummeli, Ruizhi Yang
Summary: This study proposes a solution to the commercialization problems of lithium metal batteries (LMBs) using a bifunctional Sn metal-organic framework (MOF). By utilizing SnO2 nanoparticles and molten Li infusion method, a composite Li metal anode with excellent stability and long-term performance is prepared. Additionally, Sn-MOF is added to PEO-based solid state electrolyte (SSE) to achieve a composite SSE with favorable ionic conductivity and wide electrochemical window.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Manxi Leng, Yutong Xue, Liang Luo, Xin Chen
Summary: This study investigates the corrosion inhibition performance and adsorption behaviors of imidazoline modified by different functional groups using density functional theory calculation and molecular dynamics simulation. The results show that Imidazoline-CO-CH3 and Imidazoline-CHO have the best corrosion inhibition performance. This research not only facilitates the synthesis of corrosion inhibitors with improved performance but also provides guidance for large-scale synthesis of high-efficiency corrosion inhibitors in industry.
COMPUTATIONAL AND THEORETICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jin Peng, Qiaofeng Wu, Hongming Hou, Taotao Hu, Yue Huang, Xudong Cai, Wenjie Luo, Xin Chen, Hua Yu
Summary: The power conversion efficiency (PCE) of inverted perovskite solar cells is mainly affected by the energy level mismatch and unfavorable interfacial reaction between nickel oxide (NiOx) and organic cations of the perovskite. This study introduces interlayer engineering using dual-functional alkaline hypophosphite to address these issues. The use of alkaline hypophosphite increases the valence band maximum of NiOx, aligning the energy band of perovskite solar cells with the best energy level matching using sodium hypophosphite. Additionally, the deposition of alkaline sodium hypophosphite on NiOx reduces the proportion of Ni3+, slowing down the degradation of the perovskite layer caused by the reaction with organic cations. The treated devices show improved open-circuit voltage and retain high efficiency for a prolonged period under ambient conditions, demonstrating a feasible and effective strategy for the fabrication of efficient and air-stable inverted perovskite solar cells.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Materials Science, Multidisciplinary
Yahui Li, Jingsong Tan, Xiuyun Zhao, Lei Zhao, Xin Chen
Summary: Efficient catalysts for ORR and OER are crucial in energy conversion devices. This study systematically investigates the catalytic activity of MPc-PI-COF-1 and MPc-PICOF-2 (M = Mn, Fe, Co) based on DFT methods. The results indicate that different M-N4 sites can adjust the binding strength of oxygen-containing intermediates, affecting the catalysis activity. FePc-PI-COF-1 shows exceptional resistance to poisoning.
MATERIALS TODAY COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Haiye Zhu, Yingjie Feng, Desheng Zheng, Xiuyun Zhao, Yue Zhou, Xiaoyue Fu, Lei Zhao, Xin Chen
Summary: This study reports a series of single-atom catalysts formed by nine transition metals anchored in g-C10N3, which can serve as high-performance trifunctional electrocatalysts to replace precious metal catalysts. The calculated results show that Rh@g-C10N3 and Ir@g-C10N3 have the potential to become trifunctional electrocatalysts. Furthermore, it was found that the four-electron ORR pathway on Rh@g-C10N3 is more favorable, and the *OH + H+ + e(-) -> * + H2O step has the highest energy barrier in dynamics.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
