ACS Catalysis
·
2019
·
IF 12.221
Yanfu Ma,Banlan Chi,Wei Liu,Lina Cao,Yue Lin,Xiaohui Zhang,Xuxu Ye,Shiqiang Wei,Junling Lu
Atomically dispersed metal atoms on supports, so-called single-atom catalysts (SACs), have recently attracted extensive attention in the catalysis field. It has been found that besides the primary metal atom, the proximial atoms also contribute to the catalytic activity significantly. Here, we show that tailoring of the local coordination environment of Pt1 single atoms on CeO2 using phosphorus gives rise to an activity enhancement up to a 10 times higher than Pt1/CeO2 SAC in hydrogenation of styrene, cyclohexene, phenylacetylene, and nitrobenzene. X-ray absorption, photoelectron, and infrared spectroscopies showed that the Pt1 single atoms modulated by phosphorus have a higher valence state. Infrared spectroscopy and temperature-programmed reduction further unveiled that significantly stronger adsorption of reactant and facilitated hydrogen spillover on phosphorus-doped CeO2 both play important roles for the dramatic activity enhancement. These findings point out an avenue to design an advanced SACs with high activity.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yiteng Liu,Jian Zhang,Xianxian Li,Zhaowei Zeng,Xu Cheng,Yadong Wang,Mu Pan
The investigation on highly active and durable electrocatalysts for the hydrogen evolution reaction (HER) is of great significant for renewable energy technologies. Herein, we report the fabrication of a series of amorphous Co 10-x -Ni x -B-P nanocomposites via a facile chemical reduction and phosphorization method. Compared to the Ni-B-P, Co-B-P, and other Co 10-x -Ni x -B-P electrodes, the Co 8.5 -Ni 1.5 -B-P nanocomposite catalyst exhibited the highest HER electrocatalytic activity in alkaline solution. The overpotential of Co 8.5 -Ni 1.5 -B-P is 145 mV at a current density of 10 mA cm -2 , and a low Tafel slope of 60.5 mV dec -1 is realized. Co 8.5 -Ni 1.5 -B-P also exhibits superior durability, showing no obvious degradation after 50 hours. These new phosphorous-modified borides are proved to be a new low-cost and high-efficiency catalyst system for water splitting.
研究领域:
材料科学
·
可再生能源技术
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Ling Ding,Chaoyou Tao,Shuai Zhang,Bowen Zheng,Zhenhua Dang,Lin Zhang
In this study, an amorphous silica reinforced, phosphoric-crosslinked chitosan foam (P-CTS@Si x O y ) was prepared. The introduction of amorphous silica not only increased the affinity of the adsorbent for uranium, but also improved the stability of the material. The number of active sites of P-CTS@Si x O y was increased by the introduction of phosphate groups. The material exhibited excellent uranium adsorption performance with the removal capacity and efficiency of 850.5 mg g −1 and 98.1 %, respectively. After regenerations, the morphology of P-CTS@Si x O y still maintained, and the uranium adsorption efficiency remained above 90 %, manifesting the excellent cycle performance of P-CTS@Si x O y . In the dynamic adsorption experiment, P-CTS@Si x O y successfully concentrated the volume of uranium-containing solution, and exhibited excellent uranium adsorption performance. The analysis of kinetics, isotherms, and thermodynamics manifested that the uranium adsorption behavior of P-CTS@Si x O y was a spontaneous, endothermic, monolayer chemical adsorption process. X-ray photoelectron spectroscopy, Scanning Electron Microscope, and Fourier Transform Infrared Spectrometer were used to characterized the P-CTS@Si x O y before and after adsorption, which demonstrated that the main interaction mechanism between uranium and P-CTS@Si x O y was the complexation. These studies indicated the huge application prospect of P-CTS@Si x O y in the treatment of large-scale uranium-containing wastewater.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 8
·5026-5032
·
IF 12.732
Min Liu,You Xu,Songliang Liu,Shuli Yin,Mengying Liu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
The hydrogen evolution reaction (HER) is an important process in electrochemical water splitting, and the key factor for HER technology lies in the development of cost-effective and highly efficient electrocatalysts. Herein, phosphorus (P)-modified ruthenium (Ru)–tellurium (Te) dendritic nanotubes (RuTeP NTs) are prepared via a facile two-step synthetic strategy using Te nanowires as the starting materials. The RuTeP NTs display excellent catalytic performance for the HER in alkaline media with an overpotential of only 35 mV at a cathodic current density of 10 mA cm−2, which is even superior to that of the commercial Pt/C catalyst. Detailed investigations indicate that the modification with P can improve the electrocatalytically active surface area and electron transfer capability and together with Te, modify the electronic structure of Ru atoms, which synergistically promote the HER electrocatalysis. The present work may open a new avenue to construct P-modified electrocatalysts with a rational design morphology and structure for water splitting or other electrocatalytic reactions.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2019
·
IF 7.466
Shang-Fa Pan,Jiang-Long Yin,Xue-Lian Zhu,Xiao-Jing Guo,Ping Hu,Xi Yan,Wan-Zhong Lang,Ya-Jun Guo
In this work, a variety of microporous carbon nanospheres (MCNs) were synthesized by the in-situ approach, and used as metal-free catalysts for direct propane dehydrogenation (DPDH). Pristine MCNs showed excellent catalytic performances for DPDH with initial propane conversion of 26% and propylene selectivity of 87%–88%. Phosphorus (P) modifications with different P sources put different effects on the catalytic performances of MCNs in DPDH, i.e., triethyl phosphate exhibited a positive, while (NH 4 ) 2 HPO 4 and H 3 PO 4 showed a negative effect on the catalytic performances for the in-situ doping carbon catalysts. The amount of surface oxygenic groups and the graphitization extent of carbon materials are two important factors influencing the catalytic performances of MCNs in DPDH. These results indicate that P modification is an effective way to adjust the catalytic performances of MCNs in DPDH. While, except the dopant itself, the interaction between the dopant and other materials during the synthesis process also influences the surface oxygenic groups and the graphitization degree of carbon materials.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Applied Catalysis O: Open
·
2024
·
IF 0
Yongsi Jiao,Cunjun Li,Yanqi Xu,Limei He,Linjiang Wang
Photodegradation of indigo carmine (IC) in wastewater has received much attention in recent decades. However, the current photocatalysts used for IC photodegradation suffer from an unsatisfactory efficiency due to low yield of reactive species. Herein, a P-modified biochar/g-C 3 N 4 (P-BC/CN) photocatalyst was fabricated by mechanochemical method using P-modified biochar and g-C 3 N 4 as precursors. It is discovered that P N bonds were constructed between P-modified biochar and g-C 3 N 4 , and these bonds served as the active sites to promote the generation of •O 2 − during the photodegradation process. The biochar component in P-BC/CN composite is conducive to transfer the photogenerated carriers, thereby avoiding their recombination. The photodegradation experiment showed that the P-BC/CN composite exhibits an impressive photodegradation performance towards IC ( C 0 = 50 mg/L) with a photodegradation rate of 95.3% in 120 min. This work provides a green and efficient method to design biochar-based photocatalyst with P N active sites for advanced wastewater purification.
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Huawang Zhao,Yingnan Zhao,Mengke Liu,Xianghui Li,Yuhan Ma,Xin Yong,Hong Chen,Yongdan Li
Phosphorus is introduced to modify the Cu-SSZ-13 catalyst via incipient wetness impregnation, with P/Cu-SSZ-13 = 1 and 2 wt.%, and Si/Al = 4, for selective catalytic reduction of NOx with NH 3 . N 2 physisorption and XRD results show the incorporation of phosphorus as phosphate acid enhanced the hydrothermal stability of Cu-SSZ-13 significantly, during hydrothermal aging in 10 vol.% H 2 O/air at 750 °C for 16 h. NMR and Raman results suggest that phosphate ions migrate and coordinate with the framework-bonded Al species, forming a framework silicoaluminophosphate interface, thus impeding further dealumination and structure collapse. Before the hydrothermal aging, the isolated Cu 2+ ions partly interact with the phosphate ions, forming Cu-phosphate species and reducing the SCR performance. Nevertheless, the appropriate content of phosphate ions can prevent the structure collapse caused by the hydrothermal aging, remaining the isolated Cu 2+ ions as well as excellent SCR performance.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2022
·
IF 7.129
Qiuling Yin,Peng Lyu,Guanghui Wang,Bing Wang,Yingjie Li,Zhongkui Zhou,Yadan Guo,Lianfang Li,Nansheng Deng
The decommissioning of uranium tailings (UMT) is usually accompanied by uranium (U) contamination in soil, which poses a serious threat to human health and ecological security. Therefore, the remediation of uranium pollution in soil is imminent from ecological and environmental points of view. In recent years, the use of biochar stabilizers to repair uranium tailings (UMT) soil has become a research hotspot. In this study, a novel phosphorus-modified bamboo biochar (PBC) cross-linked Mg–Al layered double-hydroxide composite (PBC@LDH) was prepared. The hyperaccumulator plant Indian mustard ( Brassica juncea L.) was selected as the test plant for outdoor pot experiments, and the stabilizers were added to the UMT soil at the dosage ratio of 15 g kg −1 , which verified the bioconcentrate and translocate of U and associated heavy metal Pb in the UMT soil by Indian mustard after stabilizer remediated. The results shown that, after 50 days of growth, compared with the untreated sample (CK), the Indian mustard in PBC@LDH treatment possessed a better growth and its biomass weight of whole plant was increased by 52.7%. Meanwhile, the bioconcentration factors (BF) of U and Pb for PBC@LDH treatment were significantly decreased by 73.4% and 34.2%, respectively; and the translocation factors (TF) were also commendable reduced by 15.1% and 2.4%, respectively. Furthermore, the Tessier available forms of U and Pb in rhizosphere soil showed a remarkably decrease compared with CK, which reached by 55.97% and 14.1% after PBC@LDH stabilization, respectively. Complexation, precipitation, and reduction of functional groups released by PBC@LDH with U and Pb described the immobilization mechanisms of biochar stabilizer preventing U and Pb enrichment in Indian mustard. As well as, the formation of U-containing vesicles was prevented by the precipitation of −OH functional groups with free U and Pb ions around the cell tissue fluids and vascular bundle structure of plant roots, thereby reducing the migration risk of toxic heavy metals to above-ground parts. In conclusion, this research demonstrates that the PBC@LDH stabilizer offers a potentially effective amendment for the remediation of U contaminated soil.
研究领域:
环境科学
·
植物学
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 14
·e202203095
·
IF 5.02
Zihan Zhou,Xingwen Wang,Junjie Li,Yu Gao,Rui Yu,Rongli Jiang
Graphical A green and efficient strategy for synthesizing phosphorus modified ZSM-5 zeolite is proposed by grinding phosphorus source, silicon source and aluminum source with the solvent-free conditions. Phosphorus-modified ZSM-5 zeolites exhibited higher light olefin selectivity and longer catalytic lifetime (33 h) in methanol to olefin reaction when the weight hourly space velocity was 4 h −1 . The traditional hydrothermal synthesis strategy of ZSM-5 zeolite is energy-consumption accompanying by pollution issues. Herein, phosphorus-modified layered ZSM-5 zeolites (PZ) were obtained by one-pot synthesis under solvent-free conditions. The synthesized samples were fully characterized by XRD, SEM, BET, NH 3 -TPD and FTIR. The effect of phosphorus addition on the morphology and catalytic activity of ZSM-5 was investigated. The results showed that phosphorus-modified ZSM-5 zeolites exhibited higher light olefin (ethylene and propylene) selectivity (above 50 %) and longer catalytic lifetime (33 h) in methanol to olefin (MTO) reaction when the weight hourly space velocity was 4 h −1 . Phosphorus-modified ZSM-5 zeolite synthesized by in situ solvent-free method, which not only reduced the discharge of sewage but also showed a simple method to realize the introduction of phosphorous species, which provided a new idea for phosphorus modification of ZSM-5 zeolite.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 6
·3086-3092
·
IF 14.511
Mei Zhang,Zhongyao Duan,Lin Cui,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Hybrid water electrolysis composed of the anodic urea oxidation reaction (UOR) and the cathodic hydrogen evolution reaction (HER) has been regarded as a green and sustainable technique for hydrogen production, and its efficiency highly depends on the identification of active electrocatalysts. Herein, a phosphorus modified mesoporous AuRh film grown on Ni foam (P-mAuRh film/NF) is synthesized via the combination of an in situ micelle assisted chemical displacement method and post phosphorization treatment process, and serves as a highly active and durable electrocatalyst for both the HER and UOR. Impressively, the self-supported P-mAuRh film/NF as both the anodic and cathodic catalyst can efficiently drive overall urea-assisted water electrolysis. The outstanding electrocatalytic performance of P-mAuRh film/NF is attributed to the synergism of the mesoporous film nanoarchitecture and optimized bimetallic composition, as well as the electron interaction between metal and nonmetal. This research offers a universal route to synthesize bifunctional nonmetal–metal mesoporous films for energy-saving H2 production via hybrid water electrolysis.
研究领域:
材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Liugen Zhang,Di Pang,Xianglei Cao,Yanfang Ma,Yuli Kou,Zechang Liu,Afaq Hassan,Changyan Guo,Fan Yue,Jide Wang
The development of efficient non-noble-metal based catalysts for oxygen evolution reaction is the crucial issue to promote electrolytic water technology. Herein, an effective phosphorus-modified hollow porous Nickel-Cobalt oxides nanocube was prepared by thermal oxidation and partial phosphorization processes. The optimal P-NiO/NiCo 2 O 4 nanocube disclosed remarkable electrochemical activity for OER in 1.0 M KOH with a low overpotential of 290 mV at 10 mA cm −2 , a low Tafel slope of 49.6 mV dec −1 , and good long-life stability for 20 h. Based on the experimental and theoretical calculation results, the introduction of P was proved to be the key to the excellent electrochemical activity for OER. P doping could optimize the adsorption of the intermediates, decrease the energy barrier and change the rate-determining step. Meanwhile, the P-dopant could modulate the electronic structure and enhance the conductivity of NiO/NiCo 2 O 4 . In addition, hollow, porous hybrid structure and oxygen vacancies could increase the number of active sites exposed, and facilitate the ion transport. The present work provides a valuable strategy to design transition-metal oxide based electrocatalysts with enhanced electrocatalytic performances by controlling partial P doping.
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
ACS Catalysis
·
2023
·
IF 12.9
Dong Ji,Peng Guo,Yongjie Xi,Jinlei Li,Jia Wang,Tingting Wang,Fuwei Li
Selective tandem hydrogenation is a promising strategy for catalytic conversion of bulk raw materials with multifunctional groups into high-value-added chemicals via multiple-step reactions. Yet now, one of the current challenges is to develop a multifunctional and stable catalyst enabling the tandem catalysis rather than interrupting at any step reaction, particularly for supported nonprecious metal catalysts. In this work, we report tandem hydrogenation of bulk phthalic anhydride toward the one-pot synthesis of hexahydrophthalide, an emerging monomer of a recyclable polyester, over phosphorus-promoted Ni–Co bimetallic alloy nanoparticle catalysts. The surface composition of catalysts can be easily regulated by changing the Ni/Co molar ratio and the phosphorous functionalization strategy, which could then tune the product selectivity and enhance the stability of this tandem process. The optimal Ni3Co1@NC-P affords 88% selectivity for the desired product and demonstrates promising stability toward the tandem hydrogenation reaction. Systematic experimental and computational studies reveal that the adsorption strength of the intermediates and the ability of hydrogen activation can be altered by the formation of surface metallic Ni species, thus tuning the product selectivity. In addition, the oxidation resistance of Ni3Co1@NC-P was enhanced by the phosphorization treatment, which makes the bimetallic alloy successfully realize the tandem hydrogenation reaction. The finding of this work not only provides a convenient strategy to design and develop efficient and stable non-noble metal-based catalysts for selective tandem hydrogenation reactions, especially involving the hydrodeoxygenation reaction, but also fulfills the straightforward pathway for the preparation of degradable polyester monomer hexahydrophthalide.
研究领域:
催化化学
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材料科学
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计算化学
✓ 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）