JOURNAL OF CATALYSIS
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2022
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IF 8.047
Jiang Li,Heyang Liu,Zhidong An,Yue Kong,Lei Huang,Delong Duan,Ran Long,Piaoping Yang,Yuan-Ye Jiang,Jiaxing Liu,Junjie Zhang,Tong Wan,Jiayi Fu,Runze Pan,Xintian Wang,Dionisios G. Vlachos
Heteroatoms-doped carbon materials have recently emerged as effective catalysts for various chemical and electrochemical reactions. The free of metals especially noble metals reduces cost and eliminates issues like sintering or leaching of metals at elevated temperatures in solvents. In this work, selective hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) is for the first time achieved over simple nitrogen-doped carbon (N-C) catalysts. At optimal reaction conditions, a 91% yield of DMF is obtained with excellent catalyst stability. Extensive characterization, including extended X-ray absorption fine-structure (EXAFS) and soft X-ray absorption spectroscopy (sXAS), model reactions, basic data science analysis, and DFT calculations suggest that ppm of Fe in particular FeN 3 sites formed in pyrolysis, rather than non-metallic elements, drive key steps such as H 2 activation and deoxygenation of –OH during HMF HDO.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 13
·7381
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IF 6.208
Daqian Wang,Zhihao Zhang,Shuchuan Xu,Ying Guo,Shifei Kang,Xijiang Chang
Defective functional-group-endowed polymer semiconductors, which have unique photoelectric properties and rapid carrier separation properties, are an emerging type of high-performance photocatalyst for various energy and environmental applications. However, traditional oxidation etching chemical methods struggle to introduce defects or produce special functional group structures gently and controllably, which limits the implementation and application of the defective functional group modification strategy. Here, with the surface carboxyl modification of graphitic carbon nitride (g-C3N4) photocatalyst as an example, we show for the first time the feasibility and precise modification potential of the non-thermal plasma method. In this method, the microwave plasma technique is employed to generate highly active plasma in a combined H2+CO2gas environment. The plasma treatment allows for scalable production of high-quality defective carboxyl group-endowed g-C3N4nanosheets with mesopores. The rapid H2+CO2plasma immersion treatment can precisely tune the electronic and band structures of g-C3N4nanosheets within 10 min. This conjoint approach also promotes charge-carrier separation and accelerates the photocatalyst-catalyzed H2evolution rate from 1.68 mmol h−1g−1(raw g-C3N4) to 8.53 mmol h−1g−1(H2+CO2-pCN) under Xenon lamp irradiation. The apparent quantum yield (AQY) of the H2+CO2-pCN with the presence of 5 wt.% Pt cocatalyst is 4.14% at 450 nm. Combined with density functional theory calculations, we illustrate that the synergistic N vacancy generation and carboxyl species grafting modifies raw g-C3N4materials by introducing ideal defective carboxyl groups into the framework of heptazine ring g-C3N4, leading to significantly optimized electronic structure and active sites for efficient photocatalytic H2evolution. The 5.08-times enhancement in the photocatalytic H2evolution over the as-developed catalysts reveal the potential and maneuverability of the non-thermal plasma method in positioning carboxyl defects and mesoporous morphology. This work presents new understanding about the defect engineering mechanism in g-C3N4semiconductors, and thus paves the way for rational design of effective polymeric photocatalysts through advanced defective functional group engineering techniques evolving CO2as the industrial carrier gas.Keywords:g-C3N4;carboxyl group;defect engineering;non-thermal plasma method;CO2utilization
研究领域:
材料科学
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光催化
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能源与环境科学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-7
·
IF 12.121
Yu Fei-Yang,Lang Zhong-Ling,Yin Li-Ying,Feng Kun,Xia Yu-Jian,Tan Hua-Qiao,Zhu Hao-Tian,Zhong Jun,Kang Zhen-Hui,Li Yang-Guang
The oxidized platinum (Pt) can exhibit better electrocatalytic activity than metallic Pt 0 in the hydrogen evolution reaction (HER), which has aroused great interest in exploring the role of oxygen in Pt-based catalysts. Herein, we select two structurally well-defined polyoxometalates Na 5 [H 3 Pt (IV) W 6 O 24 ] (PtW 6 O 24 ) and Na 3 K 5 [Pt (II) 2 (W 5 O 18 ) 2 ] (Pt 2 (W 5 O 18 ) 2 ) as the platinum oxide model to investigate the HER performance. Electrocatalytic experiments show the mass activities of PtW 6 O 24 /C and Pt 2 (W 5 O 18 ) 2 /C are 20.175 A mg −1 and 10.976 A mg −1 at 77 mV, respectively, which are better than that of commercial 20% Pt/C (0.398 A mg −1 ). The in situ synchrotron radiation experiments and DFT calculations suggest that the elongated Pt-O bond acts as the active site during the HER process, which can accelerate the coupling of proton and electron and the rapid release of H 2 . This work complements the knowledge boundary of Pt-based electrocatalytic HER, and suggests another way to update the state-of-the-art electrocatalyst.
研究领域:
电化学
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催化
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材料科学
✓ 已验证
DOI
高影响因子
CARBON
·
2025
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IF 11.6
Dan Ping,Qingshuo Zhang,Weitao Liu,Shide Wu,Jing Gao,Haoyi Zhang,Shiwen Wang,Huajun Qiu,Shaoming Fang
Electrochemical CO 2 reduction reaction (CO 2 RR) to syngas represents a promising strategy to mitigate CO 2 emission and achieve carbon neutrality. Dual-site metal catalysts have emerged as an effective candidates for syngas production, however, challenges such as limited catalytic activity and inadequate control over the H 2 /CO ratio persist. Herein, a spatially separated dual-site catalyst containing cobalt phthalocyanine (CoPc) and ∼18 nm hollow Co 3 O 4 nanoparticles (NPs) was developed, in which CoPc and Co 3 O 4 are confined outside and inside the N-doped carbon (N–C) support, respectively. Experimental and calculation analyses reveal that the CoPc sites promote CO production, while the Co 3 O 4 NPs are responsible for H 2 production. The strong electronic coupling effect among CoPc, N–C and Co 3 O 4 NPs optimizes the electronic structure of catalyst and modulates the adsorption behaviors of reaction intermediates, leading to superior catalytic performance. A consistent H 2 /CO ratio of 2:1 is achieved across an extensive potential window ranging from −0.6 to −1.1 V vs . RHE, which is highly advantageous for industrial applications. Furthermore, adjustments in catalyst composition and microenvironment enable precise tuning of the H 2 /CO ratio from 1 to 2. This study provides a straightforward approach to designing dual-site catalysts for efficient syngas production.
研究领域:
电化学
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催化
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材料科学
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环境科学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
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2021
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IF 13.084
Boyang Liu,Yu Wang,Ning Huang,Xiaocheng Lan,Tiefeng Wang
The development of a highly active heterogeneous catalyst for styrene hydroformylation is a major challenge, and we previously found that Rh2P was a good candidate. By doping a second metal of Co, we further improved the activity by 1.7 times, and the highest TOF reached 2563 h–1 on Rh7Co1P4/SiO2. The addition of Co tuned the electronic environment of surface Rh atoms without changing the crystal structure, and the reaction activity showed a volcano relationship with the Co ratio. DFT calculations showed that Co doping decreased the overall activation energy of surface reactions and destabilized H2 adsorption simultaneously. When x ≤ 2 for Rh8–xCoxP4/SiO2 catalysts, surface Rh atoms had positive valence and H2 adsorption was exothermic. Therefore, the hydroformylation rate was mainly determined by surface reaction with a first order of styrene concentration. When x > 2, however, surface Rh atoms were negatively charged and H2 adsorption became thermodynamically unfavorable. The reaction activity was then determined by H2 adsorption and was independent of styrene concentration. We introduced δE, which was the sum of overall activation energy and H2 coadsorption energy with styrene, to predict activity. Moderate addition of Co decreased the value of δE and promoted the activity, while excessive doping would increase δE.
研究领域:
化学工程
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催化
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Haiqian Lian,Eryue Song,Bin Bao,Wenhe Yang,Yu Yang,Yichang Pan,Shengui Ju
Metal-organic frameworks (MOFs) as molecular sieve membrane materials have received extensive attention on the gas separation application. However, the membrane separation performance is extremely limited by its intrinsic stability of frameworks. The successful preparation of high-quality gas separation membranes with excellent stability remains a grand challenge. ZIF-302 is based on hydrophobic ligand in-situ design with a high-stabile chabazite (CHA) topology. Herein, we synthesized uniform ZIF-302 nanocrystals with exceptional stability by introducing a modulator. Correspondingly, the continuous dense ZIF-302 polycrystalline membranes were also prepared for the separation of H 2 , N 2 , CO 2 , CH 4 and other gases. The permeance of H 2 and separation factor for H 2 /CH 4 mixtures at 35 °C and 1 bar were 2.8 × 10 -8 mol m −2 s −1 Pa −1 and 51.5, respectively, exceeding the Robeson upper bound in 2008. Furthermore, the separation performance of the super-hydrophobic ZIF-302 membranes for humidified mixed gases can maintain more than 168 h at 35 °C, indicating reliable long-term operational stability. Therefore, the CHA-type ZIF-302 polycrystalline membrane is promising for actual industrial gas separation.
研究领域:
材料科学
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化学工程
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膜技术
✓ 已验证
产品关联
DOI
高影响因子
iScience
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2023
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IF 5.8
Fuhua Xu,Jiaying Yan,Yanlan Wang,Xiang Liu
Sodium formate (SF) is regarded as a technological additive to improve H 2 generation upon HCOOH dehydrogenation. The development of SF as a hydrogen storage material is still a challenge. Herein, we report the design and synthesis of carbon nanosphere-stabilized Pd nanoparticles (Pd/CNS) for the direct H 2 generation upon SF hydrolysis in the presence of Fe 3+ . The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H 2 with one H atom provided by SF and other H by H 2 O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H 2 O and -O 2 C-H bond oxidative addition is the rate-controlling step in SF hydrolysis. This work offers a new chemical hydrogen storage material (HCOONa) for the high-efficiency generation, transport, and storage of H 2 .
研究领域:
化学
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能源科学
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催化科学
✓ 已验证
DOI
PubMed
高影响因子
MOLECULES
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2025
·Vol. 30
·期 7
·1599
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IF 4.6
Yang Li,Ying Wang,Longbo Zhang,Yanru Zhang,Jia Guo,Yanyan Wang,Chenglong Yu,Jun He,Zhenpeng Wang,Juanjuan Han,Qian Li,Tianbin Wu,Qingli Qian,Buxing Han
CO2is a greenhouse gas and a nontoxic, easily available and renewable C1feedstock. H2is a clean and cheap reductant that can be obtained from renewable energy. Olefins are platform chemicals that can be produced from a variety of raw materials such as petroleum, coal and renewable biomass. The production of carboxylic acids by combining olefins, CO2and H2is a sustainable and very promising protocol. However, only a few advances in this topic have been achieved because novel catalysts need to be developed. In this work, we demonstrate that a simple iridium-based catalyst could efficiently promote the synthesis of C2+carboxylic acids via the reaction of olefins with CO2and H2. The reaction was effectively accelerated by a simple iridium-based catalytic system at 170 °C, which may be applied to various olefin substrates. The catalytic mechanism was studied through a series of control experiments. The findings contribute to advancing the sustainable production of valuable products by the reaction of renewable CO2and green H2with platform chemicals.
研究领域:
化学催化
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可持续化学
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有机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Liu Tao,Lan Cheng,Tang Min,Li Mengxin,Xu Yitao,Yang Hangrui,Deng Qingyue,Jiang Wenchuan,Zhao Zhiyu,Wu Yifan,Xie Heping
Seawater direct electrolysis (SDE) using renewable energy provides a sustainable pathway to harness abundant oceanic hydrogen resources. However, the side-reaction of the chlorine electro-oxidation reaction (ClOR) severely decreased direct electrolysis efficiency of seawater and gradually corrodes the anode. In this study, a redox-mediated strategy is introduced to suppress the ClOR, and a decoupled seawater direct electrolysis (DSDE) system incorporating a separate O 2 evolution reactor is established. Ferricyanide/ferrocyanide ([Fe(CN) 6 ] 3−/4− ) serves as an electron-mediator between the cell and the reactor, thereby enabling a more dynamically favorable half-reaction to supplant the traditional oxygen evolution reaction (OER). This alteration involves a straightforward, single-electron-transfer anodic reaction without gas precipitation and effectively eliminates the generation of chlorine-containing byproducts. By operating at low voltages (~1.37 V at 10 mA cm −2 and ~1.57 V at 100 mA cm −2 ) and maintaining stability even in a Cl − -saturated seawater electrolyte, this system has the potential of undergoing decoupled seawater electrolysis with zero chlorine emissions. Further improvements in the high-performance redox-mediators and catalysts can provide enhanced cost-effectiveness and sustainability of the DSDE system.
研究领域:
能源科学
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环境科学
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电化学
✓ 已验证
DOI
PubMed
高影响因子
Science Bulletin
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2021
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IF 11.78
Yang Li,Xian Wang,Bingbao Mei,Ying Wang,Zhaoyan Luo,Ergui Luo,Xiaolong Yang,Zhaoping Shi,Liang Liang,Zhao Jin,Zhijian Wu,Zheng Jiang,Changpeng Liu,Wei Xing,Junjie Ge
Proton exchange membrane fuel cells (PEMFCs) suffer extreme CO poisoning even at PPM level (<10 ppm), owning to the preferential CO adsorption and the consequential blockage of the catalyst surface . Herein, however, we report that CO itself can become an easily convertible fuel in PEMFC using atomically dispersed Rh catalysts (Rh-N-C). With CO to CO 2 conversion initiates at 0 V, pure CO powered fuel cell attains unprecedented power density at 236 mW cm −2 , with maximum CO turnover frequency (64.65 s −1 , 363 K) far exceeding any chemical or electrochemical catalysts reported. Moreover, this feature enables efficient CO selective removal from H 2 gas stream through the PEMFC technique, with CO concentration reduced by one order of magnitude through running only one single cell, while simultaneously harvesting electricity. We attribute such catalytic behavior to the weak CO adsorption and the co-activation of H 2 O due to the interplay between two adjacent Rh sites.
研究领域:
能源科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
VACUUM
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2022
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IF 4.11
Hua-Dong Dong,Jian-Ping Zhao,Ming-Xing Peng,Yong-Hui Zhang,Pei-Yuan Xu
With the rise of H 2 production from water electrolysis, H 2 fuel cell and other H 2 industry, the development of H 2 detection equipment is urgent. In this work, fusiform ZnO sensitive material was synthesized by hydrothermal and photodeposition method, and Au nanoparticles were loaded on its surface by photodeposition method. The size and length of the synthesized samples are about 1 μm and 5 μm, and Au nanoparticles are evenly distributed on the surface. The XRD , FESEM, TEM and XPS characterizations of the Au-loaded ZnO (AZO) composites were collected to investigate their compositions and structures. The as-synthesized materials were applied to fabricate sensors to study their gas sensing performance. After Au modification, the H 2 sensing performance of the sensitive material is enhanced obviously. The response of AZO (Au-loaded ZnO) to 100 ppm H 2 at 230 °C is 37.6, which is 4.5 times higher than that of pure ZnO. In addition, the cross response of AZO based gas sensor to different gases was evaluated, and its sensing performance was tested for one month. The results show that AZO sensitive materials have good selectivity and long-term stability for H 2 .
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 18
·8739-8751
·
IF 3.925
Quansheng Wu,Songhua Zhou,Chengbing Fu,Jiesong Zhang,Bo Chen,Hongyan Pan,Qian Lin
For the mono-metal Pd based catalysts, the O–O bond in O2 and H2O2 is easily dissociated due to the higher energy sites of Pd, which decreases the selectivity and productivity of H2O2. To address this issue, non-noble metals M (M = Sn, Fe, Co, Ni) were doped into palladium precursors to create a series of yolk–shell structure bimetallic catalysts Pd–M@HCS (H = hollow; C = carbon; S = sphere) with Pd–M as the core and porous carbon as the shell. The results indicated that the catalyst Pd–M@HCS doped with Sn, Fe, Co, and Ni has a weak dissociation ability for O2, and both the adsorption and dissociation ability for H2 are improved. Of these catalysts, the catalyst Pd–Sn@HCS gives the best performance, which is benefited by the suitable Pd–Sn nanoparticle size and the best Pd2+/Pd0 ratio. The influence of the nPd/nSn ratio in the Pd–Sn@HCS system on catalyst performance was further explored, and the findings revealed that Pd–Sn@HCS had the best catalytic activity and stability when the nPd/nSn ratio was 2. The catalyst's H2 conversion, H2O2 selectivity, and productivity were 35%, 97%, and 3961 mmol gPd−1 h−1, respectively. After 10 cycles, the H2O2 productivity of this catalyst remained at 92.1%, which was greater than the H2O2 productivity of the typical Pd-based catalyst Pd/C, which stayed at 37% under the same conditions.
研究领域:
催化
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化学工程
·
材料科学
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）