SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yilong Zhu,Huifang Xing,Shan Ni,Ke Xu,ZhaoXiang Zhong,Liangrong Yang
The recycling of precious materials, such as palladium (Pd), was repeatedly documented as essential for a sustainable future with respect to the environment and energy production. However, high-efficiency extraction presented significant challenges. In this work, a surface hydroxyl regulation strategy was used to prepare a defective carbon nitride (CN) with a high specific surface area and hierarchical porosity through cobalt (Co)-doping. Characterization confirmed the successful synthesis of the adsorbent. The results indicated that the optimal pH for the adsorption process was 5.5, adsorption kinetics and isotherms of Pd on the adsorbent suggested that the adsorption followed a pseudo-second-order model and the Langmuir model, respectively. The maximum adsorption capacity reached up to 529.1 mg·g –1 . In addition, it showed high affinity for Pd ions, the K d value was 4.1 × 10 4 ml·g –1 . After Pd adsorption, due to the presence of abundant and uniformly dispersed Pd and Co particles which further facilitated cooperative catalysis on the surface of adsorbent, As a result, the Co-CN-Pd was reused as a catalyst for p-nitrophenol hydrogenation. It achieved a turnover frequency (TOF) as high as 1032.6 h –1 , significantly surpassing other catalysts reported in the literature. Overall, this novel adsorbent presented broad application prospects in the field of Pd recovery and reuse.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2024
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IF 14
Na Li,Tingting Ma,Huihui Wang,Jiayi Li,Dingrong Qiu,Zhen Meng,Jiangdu Huang,Lijun Sui,Faming Han,Huidan Lu,Yongping Liu,Sundaram Chandrasekaran
Rational design of defected carbons adjacent to nitrogen (N) dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon. Meanwhile, the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction (ORR) ability of inactive carbons through charge redistribution. Herein, we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the two-dimensional (2D) mesoporous N-doped carbon nanoflakes (NCNF) is a promising technique for improving ORR performance. As a result, the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts. Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site, rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR. Also, NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of ∼121.10 mW cm −2 and ∼679.86 mA h g Zn −1 , respectively. This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Lei Wang,Xuan Liu,Mengting Huang,Yun Han,Panjie Guo,Run Huang,Ying Chen,Helong Wu,Jinyan Zhang,Shuangming Chen,Aijun Du,Xin Wang
Seawater electrocatalysis is highly desired for various energy storage and conversion systems, such as water splitting using seawater as an electrolyte and metal fuel cells. However, the adsorption of chloride ions (Cl–) on the active sites of cathodes would worsen the oxygen reduction reaction (ORR) activity and stability, thus lowering the battery performance. Herein, the coupling active sites of graphitic N-regulated adjacent pentagon defects in carbon nanosheets (GAP/CN) were first synthesized by a low-boiling-point metal-mediated partial N-removal strategy. Experimental and theoretical results affirm the advantageous cooperative effect between adjacent pentagons and graphitic N toward the ORR in a harsh seawater environment, where adjacent pentagons act as the authentic highly effective ORR active sites and surrounding graphitic N site serves as the structural regulator to weaken the binding strength of harmful Cl– to prevent catalyst poisoning. As a result, GAP/CN delivers excellent ORR activities in diverse electrolytes, including 0.1 M KOH (half-wave potential of 0.87 V), alkaline artificial seawater (half-wave potential of 0.87 V), and natural seawater (half-wave potential of 0.71 V), and also good long-term stability, which can be comparable to commercial Pt/C. This study provides valuable guidance for the rational design of ORR electrocatalysts for seawater-related energy-conversion devices.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Wei Cheng,Xue Zhao,Hanyue Hu,Jiaqi Cai,Yi Wang,Xiangyang Liu,Donghui Xu,Wenxiu Luo,Guangyin Fan
The defect-rich characteristic nanostructure carbon favors the changing polarity and electron distribution in carbon matrix, thus facilitating an efficient adsorption of ions. Herein, a B,N,F-tridoped carbon material is successfully prepared on defect-rich sites by directly calcining two sodium salts, namely ethylenediaminetetraacetic acid tetrasodium salt (Na 4 EDTA) and ammonium tetrafluoroborate (NH 4 BF 4 ). B refers to electron-donating atoms while F and N are electron-accepting atoms. The co-existence of electron-donating and electron-accepting atoms causes an asymmetrical spin and charge density, favoring palladium nanoparticles (Pd NPs) well dispersed on the carbon matrix. The heteroatoms efficiently control over the growth of Pd NPs and regulate the internal electron density. The catalytic performance is significantly enhanced with the obtained Pd/BNF-C catalyst for formic acid dehydrogenation, which has a lower activation barrier (36.4 kJ/mol) and a better reusability than those of free-heteroatom catalysts. The efficiency might be attributed to the strong interaction between Pd NPs and heteroatoms, and the electrons transfer from carbon material to Pd NPs, with benefits including the significant coupling effect of B,N,F-tridoping down to the atomic scale, abundant surface active defects, in-plane nanopore defects and more adjacent metal active sites.
研究领域:
材料科学
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2018
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IF 4.439
Suyun Zhang,Xinxin Xiao,Taotao Lv,Xiaomeng Lv,Botao Liu,Wei Wei,Jun Liu
Exploring efficient and economical Pt-free electrocatalysts is of great significance for the electrocatalytic hydrogen evolution reaction (HER). However, the rational design on an industrial scale is a formidable challenge. Herein, we reported a facile calcination at controlled temperatures to fabricate rationally assembled cobalt nanoparticles embedded in defect-rich N-doped carbon nanotubes (Co-NCNTs), which was derived from low-cost dicyanadiamide thermally polymerized with cobalt precursor forming metal-organic frameworks, then further calculation leading to final products. The as-obtained samples were endowed with high content of N as electrocatalytic active site, defect-rich structure and excellent synergistic effect between cobalt nanoparticles and carbon nanotubes toward electrocatalytic HER . As expected, Co-NCNTs were highly active and long-term stable with onset potentials of c.a. 15 mV in acidic electrolytes (0.5 M H 2 SO 4 ), 70 mV in alkaline (1 M KOH) and 300 mV in neutral media (pH 7). Specially, to achieve the current density of 10 mA cm −2 , the overpotential of 103 mV in acid, 204 mV in alkaline and 337 mV in neutral media was obtained. The enhanced HER performance was discussed in detail by adjusting the molar ratio of precursor and metal species. Moreover, the present synthetic route is easy to scale up and expand to other non-noble metal and alloy.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
ACS Catalysis
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2024
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IF 11.3
Renqin Chang,Guangyu Cheng,Tao Feng,Saisai Wang,Jiale Huang,Yuchen Zhang,Chunxiao Jin,Yuxue Yue,Jia Zhao,Xiaonian Li
Porous carbon-supported quantum dot (QD) catalysts have attracted widespread attention due to their tunable energy level structure, electron transport capability, and quantum confinement effects. However, significant challenges remain in their controlled synthesis and large-scale production. To achieve this, a novel nanodigging technique (NDT) was developed for the facile synthesis of carbon-based catalysts loaded with sulfur quantum dots (S-QDs), and in situ Raman, in situ DRIFTS, and quasi-in situ X-ray photoelectron spectroscopy (XPS) techniques were performed to systematically investigated the formation mechanism of S-QDs on the carbon matrix during microwave heating. The optimal SC-600 catalysts exhibited appreciable catalytic performance in hydrochlorination of acetylene to vinyl chloride (VCM), demonstrating a high space-time yield (STY) of 23.74 kgVCM kgS–1 h–1, and durability (over 300 h). Experiment and theoretical calculations revealed that the S-QDs, in conjunction with surrounding carbon atoms, form a Frustrated-Lewis-Pair-like structure that displays significant surface charge polarization, thereby improving the selective adsorption and activation of reactants. Specifically, the p−π interactions and nonclassical hydrogen bonding effectively activate acetylene and HCl, respectively, and following a Langmuir–Hinshelwood mechanism to efficiently produce VCM. This discovery provides valuable insights into the design of carbon material surface charge distribution and spatial transfer, facilitating the targeted and controllable design and synthesis of high-efficiency QD catalysts.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 24
·19400-19406
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IF 3.201
Wei Jin,Jianping Chen
Hydrogen (H2) is an alternative clean and sustainable energy source that could alleviate the fossil fuels crisis, and eco-friendly water electrolysis has been widely employed to produce H2. Herein, we report for the first time the facile synthesis of copper(I) oxide and cobaltosic oxide hybrid nanocomposites decorating defective carbon nanotubes (Cu2O/Co3O4/DC) using a hydrothermal method. Notably, the electrocatalysis of Cu2O/Co3O4/DC is significantly improved through an electrochemical activation process. The electrochemically activated Cu2O/Co3O4/DC (ECA-Cu2O/Co3O4/DC) presents excellent HER activity and durability with a small overpotential of 160 mV at a current density of 10 mA cm−2 and a small Tafel slope of 73 mV dec−1. This high hydrogen evolution performance is attributed to the synergistic interaction between Cu2O/Co3O4 nanoparticles and defective carbon nanotubes, providing further understanding of earth-abundant transition metal-bearing electrocatalysts in emerging energy applications.
研究领域:
材料科学
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电化学
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能源技术
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
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2025
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IF 4.7
Xuan Miao,Xiao Bai,Peng Zhang,Bolong Wang,Shuyan Wang,Yuzhu Yang,Zenggang Lin,Sixia Li,Binbin Wang,Weisheng Liu
Incorporating two-phase heterojunctions with matching band structures represents a promising strategy for developing photocatalysts with enhanced efficiency. This work prefers a novel approach that employs a template-assisted strategy based on a porous structured UCCN@CeO2 0D/2D S-scheme heterojunction. The proposed method aims to improve photocatalytic activity by harnessing the synergistic effects of monodispersed CeO2 nanoparticles and ultrathin N-defect CN nanosheets. The catalyst demonstrates a remarkable photocatalytic hydrogen evolution rate, reaching an impressive value of 5.59 mmol h–1 g–1 when subjected to simulated sunlight irradiation. Furthermore, the photocatalyst maintains a substantial activity level, yielding 2.35 mmol h–1 g–1 under visible light (≥400 nm). The significant improvement in the photocatalytic performance of the UCCN@CeO2 catalyst is attributed to the unique structural design and effective charge separation facilitated by the S-scheme mechanism. Kelvin probe force microscopy, theoretical calculations, and femtosecond transient absorption spectroscopy affirm the efficient charge transportation across the catalyst interface. Additionally, electron spin resonance spectroscopy measurements further support the charge transfer pathway in the S-scheme. This research presents an innovative approach for designing and developing CN-based catalysts featuring S-scheme heterojunctions, aiming to improve their efficiency and practical use in photocatalytic applications.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Chunyu Zhang,Guozhu Liu,Bo Ning,Shuairen Qian,Danning Zheng,Li Wang
The electrochemical oxygen reduction reaction (ORR) via two-electron pathway is a sustainable way of producing hydrogen peroxide. Nanostructured carbon materials are proved to be effective catalysts for 2e − ORR. Herein, a series of mesoporous carbon with tunable nitrogen species and oxygen functional groups were synthesized by varying the added amount of dopamine hydrochloride as nitrogen and oxygen source. The modified catalysts exhibited higher content of pyrrolic-N and ether C–O groups which are confirmed by a series of characterization. Raman spectra and correlation analysis revealed that the increased proportion of defect sites in carbon materials are closely related to the introduced pyrrolic-N and ether C–O groups. And the rotating ring-disk electrode (RRDE) measurement carried out in 0.1 M KOH electrolyte showed the H 2 O 2 selectivity increased with the content of defect sites. Among them, the optimized catalyst (NOC-6M) exhibited a selectivity of 95.2% and a potential of 0.71 V vs. RHE at −1 mA cm −2 . Moreover, NOC-6M possessed the high H 2 O 2 production rate of 548.8 mmol g cat −1 h −1 with faradaic efficiency of 92.4% in a two-chamber H-cell. Further mechanistic analysis revealed that the introduction of pyrrolic-N and ether C–O are likely to improve the binding energy of the defect sites toward ∗OOH intermediate, resulting in a more favorable 2e − ORR pathway for H 2 O 2 production.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2025
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IF 11.6
Xin Xue,Bin Lou,Weiwei Pang,Shuang Han,Jichang Zhang,Jing Wu,Lingyan Tian,Nan Shi,Dong Liu
In silicon-graphite composite electrodes, the disparity in lithiation potentials between the two components exacerbates the polarization of individual components during charge/discharge processes, consequently diminishing the rate performance of the electrode materials. A robust silicon-defective carbon-graphite interface was created by coating graphite with oxidized pitch and employing surface-bonding techniques, significantly improving the rate performance and overall homogeneity of the electrode materials. The synthesized sample Si@C-MCMB exhibited the specific capacity of around 1617mAh/g at 0.1 A/g with the capacity retention of more than 85 %. In-situ XRD tests and DFT calculations reveal that due to the lower lithiation potential of graphite, it experiences a delayed discharge process within the composite anode, causing silicon to discharge independently during the initial stages of lithiation. However, the broad voltage window of defective carbon could compensate for the independent discharge behavior of silicon, promoting the homogeneity of the electrode. The faster lithium-ion diffusion in defective carbons with small graphite microcrystals and abundant defect sites also enhances the overall rate performance of the electrode materials. The study highlights using defective carbon to enhance Si-graphite composite electrodes for better battery performance, suggesting future research on optimizing the silicon-carbon interface and other carbon-based materials.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Shizhen Dong,Bin Wang,Xiaojuan Wu,Yanling Yu,Nuoxin Wang,Jinyang Li,Zuowan Zhou
This study aims to develop a universal preparation method for biomass-derived topologically defective carbons and reveal the catalytic mechanism of such carbons for cationic radical polymerization . Firstly, bamboo fiber-derived topologically defective carbon (BFTC) is prepared by an ammonia-assisted heat treatment method. BFTC can significantly promote the chemical oxidative polymerization of 3-aminophenylboronic acid (a typical cationic radical polymerization process) and obtain high molecular weight products, which is mainly attributed to the rich topological defect structure of BFTC. Secondly, the ammonia-assisted heat treatment method is applied to two other biomasses, and the derived carbons have similar microstructure and chemical composition to BFTC, indicating the universality of this method at the material preparation level; meanwhile, these derived carbons also exhibit excellent catalytic properties when they promote 3-aminophenylboronic acid (ABA) polymerization, which further confirms the universality of this method from the perspective of material properties. Finally, research on the catalytic mechanism shows that there is an interaction based on partial electron transfer between the topological defects of the carbon catalyst and ABA or ABA-derived radical. This effect promotes the rapid derivatization of ABA into cationic radical, and also improves the stability of the radical, thereby achieving efficient polymerization of ABA around the topological defect active center. Therefore, this study confirms the universality of the ammonia-assisted heat treatment method to prepare biomass-derived topologically defective carbon, and such defective carbons are likely to serve as catalysts for cationic radical polymerization .
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Hui Cai,Meng Rong,Siqi Liang,Qike Wang,Qiyu Meng,Shan Ni,Huizhou Liu,Liangrong Yang
Efficient recovery of rare earth elements (REEs) from wastewater is crucial for environmental remediation and the sustainable development of resources. Nevertheless, achieving efficient and selective REEs extraction in the systems containing low-concentration REEs and high-concentration competing metal ions remains a challenge. Here, we report on the fabrication of two-dimensional defective carbon nitride (DGCN-K) with extended nanoporous furnished oxygen-enriched sites, which is achieved through re-arrangement of framework structural unit using a flexible polycondensation-ion-thermal strategy. The extended nanoporous and continuous transmission nanochannels establish a dedicated structure microenvironment surrounding the active sites center, promoting the effective ion diffusion and increasing the accessibility of active sites. Meanwhile, the incorporation of abundant electronegative cyano and hydroxyl group modifies coordination microenvironment, improving hydrophilicity and strengthening interaction affinity with REEs. Consequently, DGCN-K shows excellent REEs adsorption performance, achieving high adsorption capacity (Nd(III) 146.25 mg/g, Dy(III) 180.82 mg/g, Lu(III) 204.34 mg/g,) within short adsorption equilibrium time (30 min). Furthermore, DGCN-K possesses high REEs selective removal rate in the mixed binary system and actual leaching tailings. This study provides a feasible microenvironment regulation strategy for the construction of 2D defective carbon nitride with oxygen-enriched sites and extended nanoporous for synergistically enabling efficient recovery of REEs.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）