CHEMISTRY OF MATERIALS
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2019
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IF 10.159
Qin Wang,Jin Li,Xianjun Tu,Hongbo Liu,Miao Shu,Rui Si,Calum T. J. Ferguson,Kai. A. I. Zhang,Run Li
Generation of efficient light-induced charge separation inside the photocatalyst is an essential factor for a high catalytic efficiency. The usual immobilization of metal or metal oxide particles on semiconductor photocatalysts offers an uncontrolled assembly of active sites during the reaction. The introduction of single metal atoms on photocatalysts can lead to extremely high atomic utilization and precise active sites. However, this approach is limited because of the lack of suitable photosensitizers for single atom immobilization. Here, we have designed photocatalytic carbon quantum dots with anchoring sites for single cobalt atoms in a defined Co–N4 structure via facile pyrolysis of vitamin B12. Carbon dots functioned as both light-harvesting antenna and support for the cobalt atom with high atom loadings up to 3.27 wt %. This new photocatalytic material demonstrated enhanced visible light absorption, efficient charge separation, and reduced electrochemical impedance, while single Co atoms acted as the active site with strong oxidative ability. As a result, the photocatalysts showed excellent visible light-promoted photocatalytic efficiency with oxygen evolution rates up to 168 μmol h–1 g–1 via water oxidation, imine formation with high conversion (∼90%) and selectivity (>99%), and complete photodegradation of organic dyes.
研究领域:
材料科学
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化学
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产品关联
DOI
高影响因子
National Science Review
·
2025
·Vol. 12
·期 3
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IF 17.1
Li Yuejiao,Li Yaguang,Shi Yushu,Gao Jianmei,Lu Jianmin,Wang Chao,Chang Junyu,Wang Zhenming,Yang Yangyue,Yang Bing,Feng Liang,Fu Qiang,Bao Xinhe,Wu Zhong-Shuai
Developing gas sensors that can simultaneously achieve high sensitivity and selectivity for the detection of a single-type gas remains a significant challenge. Herein we demonstrate cobalt (Co) single atoms with an unconventional dynamically changing coordination structure that could be used as NH3-sensing material with superior sensitivity and selectivity. According to the steric effect of 2-methylimidazole (2MI) molecules and carbonyl groups on graphene, the Co single atom is evolved into a bidentate coordinated structure (Co-2MI-G). In-situ characterization and theoretical simulation reveal that the sensing mechanism of Co-2MI-G is the specific chemical adsorption between unsaturated coordinated Co single atoms and NH3 molecules, causing a reversible switching of coordination number from 2 to 4, a valence state transfer from Co2+ to Co3+ of Co single atoms, and a band-gap width from 0.14 eV to 0.50 eV. Consequently, the Co-2MI-G-based gas sensor presents a sensing response of 67.598% for 1 ppm NH3 and a limit of detection of 2.67 ppb, at least 1.8 times higher than that of state-of-the-art NH3 sensors, together with robust stability and reproducibility. This work provides an innovative perspective on utilizing single atoms for ultra-selective gas sensing by coordination regulation.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Xue Zhao,Xue Li,Zhu Zhu,Wanbiao Hu,Haibo Zhang,Jian Xu,Xun Hu,Yingtang Zhou,Ming Xu,Hucai Zhang,Guangzhi Hu
Effective removal of pollutants that affect human health and ecosystem stability is a crucial challenge. Here, the structural confinement engineering strategy realizes the effective anchoring of atomically dispersed Co in the B-doped-CN network (BCN) (BCN/CoN[2 +2]). The advanced oxidation process (AOP) involved BCN/CoN[2 + 2] has realized the rapid and complete degradation to tetracycline (TCL), the removal of approximately 80% and 100% of tetracycline was achieved in 5 min and 30 min, respectively. The AOP with BCN/CoN[2 + 2] can degrade TCL over a wide pH; in addition, BCN/CoN[2 + 2] has the ability to efficiently degrade common pollutants, and its catalytic activity did not decay even if it was used repeated five times. Electron paramagnetic resonance (EPR) spectroscopy shows that BCN/CoN[2 + 2] drives the complete conversion of peroxymonosulfate (PMS) to 1 O 2 , and density functional theory calculations demonstrate that the base for the conversion of PMS to 1 O 2 is from the isolated state of the active site Co.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
Nano Energy
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2019
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IF 15.548
Shuai Yuan,Zonghua Pu,Huang Zhou,Jun Yu,Ibrahim Saana Amiinu,Jiawei Zhu,Qirui Liang,Jinlong Yang,Daping He,Zhiyi Hu,Gustaaf Van Tendeloo,Shichun Mu
The development of a stable, efficient and economic catalyst for hydrogen evolution reaction (HER) of water splitting is one of the most hopeful approaches to confront the environmental and energy crisis. A two-step method is employed to obtain metal clusters (Ru, Pt, Pd etc.) combining single cobalt atoms anchored on nitrogen-doped carbon (Ru/Pt/Pd@Co-SAs/N-C). Based on the synergistic effect between Ru clusters and single cobalt atoms, Ru@Co-SAs/N-C exhibits an outstanding HER electrocatalytic activity . Specifically, Ru@Co-SAs/N-C only needs 7 mV overpotential at 10 mA cm -2 in 1 M KOH solution, which is much better than commercial 20 wt% Pt/C (40 mV) catalyst. Density functional theory (DFT) calculations further reveal the synergy effect between surface Ru nanoclusters and Co-SAs/N-C toward hydrogen adsorption for HER. Additionally, Ru@Co-SAs/N-C also exhibits excellent catalytic ability and durability under acidic and neutral media. The present study opens a new avenue towards the design of metal clusters/single cobalt atoms heterostructures with outstanding performance toward HER and beyond.
研究领域:
材料科学
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催化化学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
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2022
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IF 8.047
Feiying Tang,Guangji Zhang,Liqiang Wang,Jianhan Huang,You-Nian Liu
Engineering unsymmetrical coordination is an efficient strategy for improving the performance of carbon supported single-atom catalysts for diverse applications. However, the exploration of this strategy to prepare carbon supported single-atom catalysts for hydrogenation reaction is still in infancy, especially for hydrogenation of quinolines. Herein, we report a protein-metal-ion-network strategy for preparation of single-atom cobalt supported on hierarchically porous carbon (SA-Co/NSPC). SA-Co/NSPC features unsymmetrically N/S-coordinated metal center, i.e., Co 1 –N 3 S 1 . Moreover, the carbon matrices possess an ultra-thin two-dimensional morphology and hierarchically porous structures. SA-Co/NSPC catalyst with Co 1 –N 3 S 1 active site exhibits excellent catalytic performance for hydrogenation of N-heterocycles. The DFT calculation results show that the site of Co 1 –N 3 S 1 reveals a significant electron redistribution in comparison to the Co 1 –N 4 , leading to a lower H* diffusion barrier and quinoline hydrogenation reaction barrier. SA-Co/NSPC catalyst combined with the unique hierarchically porous structure and high active Co 1 –N 3 S 1 owns extraordinary catalytic performance for hydrogenation of quinolines.
研究领域:
催化化学
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材料科学
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理论计算
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Wenxiu Li,Wei Li,Zanwu Guo,Yi Song,Shaoru Tang,Yanan Ma,Xueqing Xing,Qian Wang
The atomically thin nanosheets of graphitic carbon nitride (g-C3N4) with mesopores have been successfully exfoliated with supercritical CO2 (scCO2). The thickness of the as-synthesized samples could be directly tailored by simply regulating the scCO2 pressure. The obtained bilayer mesoporous g-C3N4 nanosheets doped with monatomic Co through a microwave-assisted approach havve been employed as single-atom catalysts to enhance the photocatalytic hydrogen evolution performance. The as-prepared Co/P/CN-sc sample exhibited a boosted H2 production performance due to its unique structural advantages by exposing more active sites and facilitating the separation of charge carriers. Based on X-ray photoelectron spectroscopy, steady-state and time-resolved photoluminescence spectroscopy, X-ray absorption fine structure measurement, and density functional theory (DFT) calculations, a possible mechanism has been proposed. The work shows a new perspective for designing an inexpensive photocatalyst with a unique structure through a facile and green approach for photocatalytic hydrogen evolution.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
PubMed
高影响因子
Chem
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2023
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IF 23.5
Jie Ding,Zhenyuan Teng,Xiaozhi Su,Kosaku Kato,Yuhang Liu,Ting Xiao,Wei Liu,Lingyue Liu,Qiao Zhang,Xinyi Ren,Jincheng Zhang,Zhaoyang Chen,Ohno Teruhisa,Akira Yamakata,Hongbin Yang,Yanqiang Huang,Bin Liu,Yueming Zhai
By breaking structural symmetry of the single atomic active site, the photocatalytic water oxidation pathway is tuned for highly selective oxidation of CH 4 to CH 3 OH in an aqueous solution. The water oxidation ability and its influence on photocatalytic oxidation of CH 4 over symmetrically coordinated cobalt single atom (Co-4N) on carbon nitride (SC-Co 1 /PCN) and asymmetrically coordinated cobalt single atom (Co-C2N2) on carbon nitride (AC-Co 1 /PCN KOH ) photocatalysts are systematically investigated. A super selectivity of 87.22% for photocatalytic oxidation of CH 4 to CH 3 OH is realized on AC-Co 1 /PCN KOH , which is only 45% on SC-Co 1 /PCN. Moreover, a CH 4 conversion of 2.42% and a CH 3 OH yield of 2.11% are achieved over AC-Co 1 /PCN KOH (200 mg). Combining multiple in-situ characterizations and time-dependent density functional theory calculations, it is revealed that AC-Co 1 /PCN KOH possesses a desired electronic configuration for single-electron transfer water oxidation reaction during photocatalysis, leading to a notably promoted selectivity for CH 4 oxidation to CH 3 OH under illumination.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2024
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IF 4.3
Yuhang Huang,Qihao Shen,Yahong Pu,Junyi Yu,Yu Xiong,Tao Gan,Lei Tao,Jian Zhang,Xianfeng Huang
Heterogeneous catalysts are fascinating for advanced oxidation processes (AOPs) in wastewater treatment to reduce cost, metal contamination, and pH operation limitations. However, they usually encounter low catalytic efficiency because of the difficult single-electron-transfer (SET) pathway during AOPs. Herein, an efficient heterogeneous catalyst for AOPs is realized through the rational regulation of N coordination around Co single-atom (SA) centers in favor of SET. As guided by calculations, low N coordination enables a high density of electronic states at the Fermi energy level of SA Co to facilitate SET activation of peroxomonosulfate (PMS). A special oxide-compounding method is further applied to decrease the N coordination of SA Co on the carbon carriers from common Co1–N3/4 to the desired Co1–N2. Co1–N2 shows a delightful activity for AOP degradation of various organic pollutants with kinetic rate and turnover frequency values up to 0.862 min–1 and 389 h–1, respectively, greatly outperforming those of Co1–N3/4. It is also superior in a wide pH operation range and has strong resistance to environmental disturbances. Detailed mechanistic investigations confirm the generation of singlet oxygen (1O2) instead of common radical O species from the SET between PMS and Co1–N2, corroborating the calculated results and accounting for the enhanced AOP activity.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yunhe Li,Ming Yi,Jiangwei Shang,Yilong Hou,Shengwen Zhou,Xiuwen Cheng
Singlet oxygen ( 1 O 2 ) is an excellent reactive species with solid resistance to refractory pollutants, and it is critical to enhancing the generation of 1 O 2 in the persulfate system. In this work, we developed a vacancy-containing copper oxide supported Co single atom catalyst (Co SACs /CuO(O v )) containing abundant cobalt active sites for the activation of PMS to achieve efficient 1 O 2 selective generation, thereby exhibiting ultra-high ciprofloxacin removal efficiency. Density functional theory calculations revealed that Co SACs /CuO(O v ) adsorbed the single O atom from the SO 4 side chain of PMS, facilitating its oxidation into *OH and subsequent efficient production of 1 O 2 . The Co SACs /CuO(O v )/PMS system exhibited strong resistance to variations in pH and coexisting substances in water, and the toxicity of CIP was significantly reduced after treatment. Furthermore, when the Co SACs /CuO(O v ) catalyst was immobilized on the PTFE filter membrane, it maintained the CIP removal efficiency above 75 % for 20 h under low temperatures (0℃) and in various complex aqueous environments. This work provides new insights into the design of catalysts featuring single-atom active sites and high-efficiency 1 O 2 generation, which is essential for potential applications in water purification.
研究领域:
环境科学
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催化化学
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水处理技术
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Baocang Liu,Yan Cheng,Bo Cao,Minghao Hu,Peng Jing,Rui Gao,Yaping Du,Jun Zhang,Jinghai Liu
A multicomponent 3D monolithic electrode was designed that consists of Co single atoms anchored/nitrogen, sulfur co-doped carbon nanotubes (CoSAs-NS-CNTs) on carbon cloth (CC) with ultra-thin MoS 2 nanosheets externally decorated and ultra-small CoS 2 nanodots internally confined (MoS 2 /CoSAs-NS-CNTs@CoS 2 /CC) to form a hybrid heterojunction electrode with double interfaces as vectorial electron transport pathways for promoting electrocatalytic performance. The integration of well-distributed MoS 2 nanosheets and CoS 2 nanodots linked with Co single atoms anchored/N, S co-doped CNTs endows abundant multiple active sites, outstanding conductivity, and the downshifted d-band center with a thermodynamically favorable hydrogen adsorption free energy (ΔG H* ) for effectively catalyzing hydrogen evolution reaction (HER). As a result, the optimal MoS 2 /CoSAs-NS-CNTs@CoS 2 /CC electrode exhibits outstanding HER performance with overpotentials of 72 and 56 mV at 10 mA cm −2 and small Tafel slopes of 59.4 and 43.2 mV dec -1 in acidic and alkaline solutions, respectively, outperforming most of the previously reported molybdenum/cobalt sulfide-based electrocatalysts. Moreover, the electrode also displays good durability and stability reflected from the small decrease on activity after 5000 CV cycles and nearly no decay in current density after electrolysis for 20 h.
研究领域:
材料科学
·
电催化
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Meng Xie,Mingya Yao,Shiyong Zhang,Lingshuai Kong,Lingxi Zhao,Jinhua Zhan,Ru-Song Zhao
Carbon-based single-atom cobalt catalysts exhibit high catalytic activity for the removal of novel pollutants in advanced oxidation processes. Here, atomically dispersed Co species with five-coordinated nitrogen atoms on carbon nanotubes (CNT) catalyst (Co-N 5 /CNT) was successfully fabricated via a low-temperature solvothermal reaction. The obtained Co-N 5 /CNT catalyst exhibited superior catalytic performance for PMS activation for sulfamerazine degradation. Its apparent rate constant k obs was 1.6 times higher than that of the Co-N 4 /CNT catalyst with four-coordinated nitrogen atoms prepared by the same method. Electron transfer non-radical mechanism was the main pathway for Co-N 5 /CNT to activate PMS. Higher single-atom cobalt metal loading (1.39 wt% vs 1.08 wt% in Co-N 4 /CNT) and significantly enhanced electron transfer ability (0.82 e vs 0.77 e in Co-N 4 /CNT) were the key factors for its superior catalytic performance. This work demonstrates a novel carbon-based single-atom cobalt catalyst for the removal of novel antibiotic contaminants by activating PMS in environmental catalysis applications.
研究领域:
环境催化
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材料科学
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污染治理
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Shenfei Zhao,Xiaoshuai Wu,Jiliang Zhang,Chunjie Li,Zixiang Cui,Weihua Hu,Ruguang Ma,Changming Li
Aqueous zinc-sulfur batteries at room temperature hold great potential for next-generation energy storage technology due to their low cost, safety and high energy density. However, slow reaction kinetics and high activation energy at the sulfur cathode pose great challenges for the practical applications. Herein, biomass-derived carbon with single-atomic cobalt sites (MMPC-Co) is synthesized as the cathode in Zn-S batteries. The catalysis of single-atom Co sites greatly promotes the transform of cathode electrolyte interface (CEI) on the cathode surface, while offering accelerated charge transfer rate for high conversion reversibility and large electrochemical surface area (ECSA) for high electrocatalytic current. Furthermore, the rich pore structure not only physically limits sulfur loss, but also accelerates the transport of zinc ions. In addition, the large pore volume of MMPC-Co is able to relieve the stress effect caused by the volume expansion of ZnS during charge/discharge cycles, thereby maintaining the stability of electrode structure. Consequently, the sulfur cathode maintains a high specific capacity of 729.96 mA h g −1 after 500 cycles at 4 A g −1 , which is much better than most cathode materials reported in the literature. This work provides new insights into the design and development of room-temperature aqueous Zn-S batteries.
研究领域:
材料科学
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能源存储技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）