Article
Chemistry, Physical
Siqi Yu, Qin Wang, Jianwei Wang, Yong Xiang, Xiaobin Niu, Tingshuai Li
Summary: In this study, Fe2O3 nanoparticles doped with zinc were proposed as an efficient electrocatalyst for converting N-2 to NH3. The catalyst showed high Faradaic efficiency, large NH3 yield rate, excellent selectivity, and stability in neutral media. Theoretical calculations suggested a low energy barrier for the reaction, following an associative enzymatic mechanism.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Nanoscience & Nanotechnology
Yingying Dong, Tao Wang, Shui Hu, Ying Tang, Xiaotong Hu, Yaoyao Ye, Hui Li, Ding Cao
Summary: The study demonstrates the efficient conversion of N2 into NH3 using Ag-doped titanium dioxide nanofiber catalyst synthesized by electrospinning. The catalyst showed high NH3 yield rates and stability, indicating its potential as a high-performance ENRR catalyst.
ACS APPLIED NANO MATERIALS
(2021)
Article
Chemistry, Inorganic & Nuclear
Yu Wang, Rui-Cheng Qin, Dan Wang, Chun-Guang Liu
Summary: In this study, a homo-nuclear dual-atom catalyst consisting of tantalum anchored onto a mono-tantalum-substituted Keggin-type polyoxometalate support was developed for nitrogen reduction reaction. Density functional theory calculations revealed that the metal-support interaction of the catalyst was mainly determined by bonding interaction, and the catalyst possessed suitable molecular orbitals for N-2 activation. The unique structural and electronic properties of the catalyst were found to enable effective electron transfer and reduce the free energy barriers for N-2 reduction to ammonia.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Lijuan Niu, Dandan Wang, Kang Xu, Weichang Hao, Li An, Zhenhui Kang, Zaicheng Sun
Summary: Experimental and theoretical studies have shown that V-doped MoS2 exhibits better nitrogen adsorption and activation, while Fe-doped MoS2 achieves the highest ammonia yield in experiments. Thus, achieving an appropriate balance between nitrogen adsorption, activation, and desorption is crucial for obtaining highly efficient electrocatalysts for NRR.
Article
Chemistry, Inorganic & Nuclear
Haijun Chen, Jie Liang, Kai Dong, Luchao Yue, Tingshuai Li, Yongsong Luo, Zhesheng Feng, Na Li, Mohamed S. Hamdy, Abdulmohsen Ali Alshehri, Yan Wang, Xuping Sun, Qian Liu
Summary: In this study, a hybrid catalyst of TiO2 and juncus effusus-derived carbon microtubes with a three-dimensional cross-linked hollow tubular structure is proposed for efficient electrocatalytic conversion of N-2 to NH3 at ambient conditions. The catalyst shows a high NH3 yield and faradaic efficiency in 0.1M Na2SO4, along with superior electrochemical and structural stability.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Yu Zou, Lu Wen, Xiaoqiong Bian, Yongfan Zhang, Wei Lin, Shuping Huang, Kaining Ding
Summary: Based on density functional theory calculations, it was found that Mo atoms serve as the real active sites in the MoFeS4/GR catalyst, allowing for nitrogen fixation with good selectivity. Charge was identified as the main factor affecting the catalyst's nitrogen fixation activity. The role of Mo atoms is to provide electrons while Fe atoms transport electrons in the catalyst.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Huiru Yang, Dan Luo, Rui Gao, Dandan Wang, Haibo Li, Zhao Zhao, Ming Feng, Zhongwei Chen
Summary: Electrochemical techniques for ammonia synthesis are considered promising for achieving nitrogen cycle balance. The study reveals that Ni clusters supported on TiO2 can serve as efficient catalysts for N-2 reduction, providing multiple active sites for N-2 adsorption and activation. This work identifies the potential-limiting steps in the nitrogen reduction reaction and suggests strategies for constructing efficient catalysts for NRR and NH3 synthesis using metal oxide supported transition metal clusters.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Xing-Qi Han, Zhong-Ling Lang, Feng-Yi Zhang, Hong-Liang Xu, Zhong-Min Su
Summary: Fe-Mo system is considered the most successful nitrogenase system in synthesizing ammonia, with Fe or Mo playing key roles in nitrogen reduction reaction (NRR). By incorporating Fe-Mo atoms on 2D materials, Fe-Mo supported on C2N is found to be the most promising NRR catalyst, showing superior performance and excellent selectivity. The high NRR activity of FeMo@C2N is attributed to the high localized electronic states near the Fermi level, providing optimal electronic state for Fe-Mo active sites.
APPLIED SURFACE SCIENCE
(2022)
Article
Electrochemistry
Kai Li, Yan Li, Kun Jiang, Tao Li, Yun-Quan Liu, Shuirong Li, Duo Wang, Yueyuan Ye
Summary: The dual-metal MoFe compound catalyst with tetravalent Mo active sites significantly improved the FE in NRR; the prepared MoFe-N catalyst showed a remarkable 33.26% FE and a NH3 yield rate of 33.31μg h(-1) mg(-1); thermal processing under NH3 atmosphere formed Mo(IV) active sites, leading to a significant suppression of HER activity.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Wenjing Li, Yuqing Deng, Li Luo, Yeshuang Du, Xiaohong Cheng, Qi Wu
Summary: An efficient porous nanoblock catalyst N-doped Fe2O3/NiTe2 heterojunction for overall water splitting is reported. The 3D self-supported catalysts exhibit good hydrogen evolution reaction (HER) activity and oxygen evolution reaction (OER) properties in alkaline solution. It achieved a current density of 10 mA cm-2 under 1.54 V with good durability (at least 42 h) when used as a dual function catalyst with overall water splitting.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Tingshuai Li, Jiaojiao Xia, Qiru Chen, Ke Xu, Yang Gu, Qian Liu, Yonglan Luo, Haoran Guo, Enrico Traversa
Summary: In this study, monodisperse Cu clusters loaded on defective ZrO2 nanofibers were used as an electrocatalyst for nitrogen reduction, achieving high NH3 yield rate and optimal Faradaic efficiency. Density functional theory calculations revealed that N-2 molecule was reduced to NH3 at Cu active site with an ideal overpotential. The interaction between bonding and antibonding of Cu-N bond promoted activation of N-2 and maintained a low desorption barrier.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Tingshuai Li, Jiaojiao Xia, Haohong Xian, Qiru Chen, Ke Xu, Yang Gu, Yonglan Luo, Qian Liu, Haoran Guo, Enrico Traversa
Summary: In this study, it is reported that Fe ion grafted on MoO3 nanorods can enhance the electron harvesting ability and the selectivity of H+ during the nitrogen reduction reaction in neutral electrolyte. The electrocatalyst showed remarkable ammonia yield and Faradaic efficiency under experimental conditions.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Nanoscience & Nanotechnology
Jimin Kong, Min-Seok Kim, Ramavi Akbar, Hee Young Park, Jong Hyun Jang, Hansung Kim, Kahyun Hur, Hyun S. Park
Summary: The Fe-CuS/C catalyst exhibits a high NH3 production rate in the nitrogen reduction reaction, but rapid degradation of the catalyst hinders precise investigation in longer measurements. However, when the degradation effect is mitigated, the NH3 production rate is enhanced with increased overpotentials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Bingling He, Peng Lv, Donghai Wu, Xue Li, Rui Zhu, Ke Chu, Dongwei Ma, Yu Jia
Summary: Electrocatalytic NO reduction reaction (NORR) to NH3 is a promising method for simultaneous NO removal and NH3 synthesis. This study demonstrates that angstrom-size single atomic vacancies (SAVs) can enhance the selectivity of NO-to-NH3 conversion. Aliovalent ion doping can also optimize the activity and stability of NORR.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Nanoscience & Nanotechnology
Atul Verma, Esakkinaveen Dhanaraman, Wen-Ting Chen, Yen-Pei Fu
Summary: Photocatalytic N-2 fixation is a complex reaction, which requires the design and analysis of highly efficient materials. In this study, one-pot hydrothermal Bi2WO6-BiOCl heterojunctions were synthesized by adjusting the molar ratio of tungsten and chlorine precursor. The formation of a p-n heterojunction between Bi2WO6 and BiOCl resulted in a reduction of the work function and improved catalytic performance.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Environmental
You-Gan Wang, Qing-Hua Hu, Juan Huang, Wei Jiang, Li Zhang, Ru-Ping Liang, Jian-Ding Qiu
Summary: The design of anion-scavenging materials with high charge density and accessible adsorption sites is crucial for the removal of anions, such as 99TcO4-, from radioactive nuclear waste. In this study, a cationic organic polymer called TrDCPN was synthesized to efficiently trap perrhenate (ReO4-), serving as a surrogate for 99Tc. The TrDCPN demonstrated excellent affinity towards ReO4- even in the presence of competitive anions, and it exhibited promising reusability for trapping ReO4-. The introduction of halogen in the synthetic cationic organic polymer effectively enhanced its adsorption capacity, making it a promising solution for removing radioactive pollutants from the environment.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Cheng-Rong Zhang, Jia-Xin Qi, Wei-Rong Cui, Xiao-Juan Chen, Xin Liu, Shun-Mo Yi, Cheng-Peng Niu, Ru-Ping Liang, Jian-Ding Qiu
Summary: Researchers have developed a stable carbon material for extracting uranium from seawater. This material demonstrates high selectivity and fast kinetics for uranium adsorption, as well as excellent stability and optoelectronic properties for uranium electroextraction. This work expands the application prospects of functionalized 3D carbon materials and provides technical support for electrodeposition adsorption of uranium from seawater.
SCIENCE CHINA-CHEMISTRY
(2023)
Article
Chemistry, Analytical
Xi-Rui Deng, Sheng-Qian Hu, Chen Sun, Sai-Jin Xiao, Gui-Ping Yang, Qiong-Qing Zheng, Ru-Ping Liang, Li Zhang, Jian-Ding Qiu
Summary: This study proposes a novel in-situ strategy to construct uracil-conjugated COFs with tunable fluorescence properties for sensitive and selective mercury(II) detection. By changing the molar ratio of precursors, the crystalline structure, fluorescence properties, and sensing performance of COFs can be regulated. This research opens up a new strategy for the effective and controllable construction of functionalized COFs for environmental analysis.
ANALYTICA CHIMICA ACTA
(2023)
Article
Chemistry, Analytical
Li Zhang, Quan-Gen Tan, Sai-Jin Xiao, Gui-Ping Yang, Xin Liu, Qiong-Qing Zheng, Jia-Qi Fan, Ru-Ping Liang, Jian-Ding Qiu
Summary: In this work, a photosensitive covalent-organic framework (TphBT) was synthesized and its oxidase and peroxidase activities were reversely regulated by surface modification of single-stranded DNA (ssDNA) for the colorimetric detection of UO22+.
ANALYTICAL CHEMISTRY
(2023)
Article
Engineering, Environmental
Xin Liu, Rui-Xiang Bi, Cheng-Rong Zhang, Qiu-Xia Luo, Ru-Ping Liang, Jian-Ding Qiu
Summary: Uranium removal by photocatalytic reduction is effectively achieved using a Z-scheme van der Waals heterojunction photocatalyst (SnS2COF) synthesized by combining covalent organic frameworks (COF) with semiconductor (SnS2). The SnS2COF heterojunction exhibits superior U (VI) reduction capacity in rare earth tailings wastewater due to wider light absorption range, more active sites, and higher electron-hole separation and transfer efficiency. Under photoexcitation, the heterojunction maintains high reducibility and avoids photocorrosion of SnS2. The organic-inorganic heterojunction design concept provides an alternative strategy to enhance photocatalytic performance.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Shanshan Yu, Chuangye Li, Zifan Li, Fangru Song, Zhenzhen Xu, Yean Zhu, Chunhui Dai, Xiaohong Cao, Zhibin Zhang, Yunhai Liu, Jianding Qiu
Summary: Three novel full-spectrum responsive biomimetic donor-acceptor conjugated microporous polymers were successfully constructed to efficiently photoreduce uranium. The optimized polymers exhibited narrow band gaps, stronger built-in electric fields, and efficient charge separation, achieving a high photocatalytic U(VI) reduction efficiency. This work provides a novel approach for designing high-performance green biomimetic photocatalysts for removing radioactive pollution.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Chemical
Run-Han Yan, Wei-Rong Cui, Wei Jiang, Juan Huang, Ru-Ping Liang, Jian-Ding Qiu
Summary: In this work, a covalent polymeric network (Py-CPN) based on pyridinium was successfully designed and synthesized, which showed high efficiency and reliability in adsorbing radioactive 99TcO4. This research has significant implications for environmental protection.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Engineering, Chemical
Xiao-Rong Chen, Cheng-Rong Zhang, Wei Jiang, Xin Liu, Qiu-Xia Luo, Li Zhang, Ru-Ping Liang, Jian-Ding Qiu
Summary: In this study, a novel three-dimensional cationic covalent organic framework (TFAM-BDNP) was designed and synthesized via Zincke reaction for the selective capture of TcO4-/ReO4-. TFAM-BDNP exhibited high adsorption capacity and extremely fast exchange kinetic for ReO4-, attributed to its open 3D hydrophobic channels, abundant active sites, and high chemical stability. Furthermore, TFAM-BDNP showed good adsorption performance for ReO4- in the presence of competing anions and under a wide pH value range, indicating its potential for efficient capture of TcO4-/ReO4- in complex environmental systems.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Engineering, Chemical
Yu-Zhen Shi, Qing-Hua Hu, Xin Gao, Li Zhang, Ru-Ping Liang, Jian-Ding Qiu
Summary: An indium-based metal-organic framework (In-MOF) is reported for highly efficient removal of radioactive iodine from seawater. In-MOF shows high chemical stability, high adsorption capacity, and high selectivity towards iodine, leading to a high removal rate of 93.86% from seawater.
SEPARATION AND PURIFICATION TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Li Zhang, Quan-Gen Tan, Sai-Jin Xiao, Gui-Ping Yang, Qiong-Qing Zheng, Chen Sun, Xiang-Lan Mao, Jia-Qi Fan, Ru-Ping Liang, Jian-Ding Qiu
Summary: A covalent organic framework (Tph-BT COF) with excellent photocatalytic activity is constructed by Schiff base reaction, and its mimetic oxidase and peroxidase activities are inversely regulated by single-stranded DNA (ssDNA). Under LED light irradiation, Tph-BT exhibits outstanding oxidase activity, which is inhibited by ssDNA with poly-thymidine (T) sequences, while its weak peroxidase activity is enhanced by ssDNA with poly-cytosine (C) sequences. The study also investigates the influence of base type, base length, and other factors on the activities of the two enzymes, revealing the mechanisms behind the regulation by ssDNA.
Article
Chemistry, Multidisciplinary
Qiao-Qiao Jiang, Ya-Jie Li, Qiong Wu, Ru-Ping Liang, Xun Wang, Rui Zhang, Ying-Ao Wang, Xin Liu, Jian-Ding Qiu
Summary: A creative lock-key model based on molecular insertion strategy was used to construct molecular-inserted covalent organic frameworks, allowing for the smart modulation of photoelectric responses. This approach avoids the arduous selection and synthesis conditions required by conventional COFs, providing a promising direction for the construction of late-model photoelectric responsive materials.
Article
Spectroscopy
Sai Jin Xiao, An Ting Qiu, Hui Han Li, Meng Ping Wang, Li Zhang, Kai Xin Guo, Jing Guo, Jian-Ding Qiu
Summary: In order to ensure the long-term sustainable development of nuclear energy and prevent uranium pollution, there is an urgent need for new materials that can detect and separate uranium simultaneously. In this study, a new fluorescent covalent organic polymer (COP) named HT-COP-AO was synthesized and used as a fluorescent probe and absorbent for uranium detection and separation. The results showed that HT-COP-AO had a strong fluorescence quenching effect on uranium with a detection limit of 0.23 μM. It was found that uranium was coordinated with the amidoxime groups of HT-COP-AO through U-N and O = U = O bonds, leading to electron transfer and fluorescence quenching.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2023)
Article
Chemistry, Analytical
Xiang-Lan Mao, Qiu-Xia Luo, Yuan-Jun Cai, Xin Liu, Qiao-Qiao Jiang, Cheng-Rong Zhang, Ru-Ping Liang, Jian-Ding Qiu
Summary: The isomerism of a covalent organic framework (COF) greatly affects its electrochemiluminescence (ECL) performance. In this study, two isomeric COFs, TFPB-BD(OMe)(2)-H and TAPB-BD(OMe)(2)-H, were synthesized based on different imine linkages and conversion to the quinoline structure. Despite having the same composition and similar structures, the two COFs exhibited significant differences in photoelectrochemical and ECL fields. TFPB-BD(OMe)(2)-H showed a superior ECL emission compared to TAPB-BD(OMe)(2)-H due to stronger polar interaction and enhanced electron interactions.
ANALYTICAL CHEMISTRY
(2023)
Article
Engineering, Environmental
Xin Gao, Qing-Hua Hu, Yu-Zhen Shi, Ru-Ping Liang, Jian-Ding Qiu
Summary: Here, we report a new adsorbent named Zn-Vlm6 with highly selective and high adsorption capacity for removing I3- from water. Zn-Vlm6 showed excellent thermal and chemical stability and achieved a high adsorption capacity of 1680.7 mg g-1 for I3-. It can selectively capture I3- in the presence of competing anions and remove up to 96.4% of I3- from different environments. Moreover, Zn-Vlm6 can also adsorb gaseous iodine up to 2470 mg g-1.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Xiao-Rong Chen, Cheng-Rong Zhang, Xin Liu, Ru-Ping Liang, Jian-Ding Qiu
Summary: A novel fluorescent ionic covalent organic framework (BTTA-BDNP) based on a linked carbazole unit was developed for the simultaneous monitoring and capture of TcO4-/ReO4-. BTTA-BDNP demonstrated a rapid fluorescence response with a low detection limit (66.7 nM) for ReO4- (a non-radioactive substitute for TcO4-). Moreover, BTTA-BDNP exhibited excellent selectivity and efficiency in trapping ReO4- in complex environments due to its high charge density and hydrophobic skeleton.
CHEMICAL COMMUNICATIONS
(2023)
