Green Chemical Engineering
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2024
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IF 9.1
Ruichang Xue,Rongrong Deng,Yan Li,Mengqiu Gao,Jiafu Wang,Qibo Zhang
Developing electrocatalysts with excellent activity, high stability, and low cost is vital for large-scale hydrogen production through electrochemical water splitting. Herein, a bifunctional Ni–Fe–P catalyst in situ grown on Fe foam (Ni–Fe–P/FF) is developed by a simple one-step solvothermal process in the deep eutectic solvent (DES) of ethylene glycol and choline chloride (named Ethaline). The unique solvent environment of Ethaline assisted with the regulating effect of the introduced Fe(III) ions shows an essential role in governing the preparation process. The developed Ni–Fe–P/FF acts as the efficient bifunctional electrocatalyst for water splitting in 1.0 M KOH, requiring overpotentials of 82 mV (229 mV) and 263 mV (370 mV) to deliver 10 mA cm −2 (100 mA cm −2 ) for oxygen and hydrogen evolution reactions, respectively. Furthermore, the self-supported catalyst-assembled electrolyzer also exhibits good catalytic performance with a low voltage of 1.83 V to drive 100 mA cm −2 and good stability over 100 h. This work offers a facile approach to fabricating high-performance bifunctional Ni–Fe–P electrocatalysts to catalyze water splitting.
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yijie Yang,Yanjun Yu,Yuanhang Wu,Hongyi Chen,Jie Yang,Yu Luo,Yuan Hu,Congshu Huang,Hui Li,Jianzhi Wang
Designing ultrahigh energy density and mass-loading of electrocatalysts for hydrogen evolution is highly desirable but remains a great challenge. Herein, a 3D high-rise architectural structure consisting of dense Ni(OH) 2 nanoparticles on CuMoO 4 nanocube heterostructure arrays on Ni foam (Ni(OH) 2 /CuMoO 4 /NF) is developed via a hydrothermal reaction, calcination and electrodeposition method. Benefitting from the optimized electronic configuration, hierarchical high-rise architecture, and large specific surface area and mesoporous, the Ni(OH) 2 /CuMoO 4 /NF exhibits superior hydrogen evolution reaction (HER) activity in 1.0 M KOH solution. Ni(OH) 2 /CuMoO 4 /NF only requires low overpotential of 70 mV achieving a current density of 10 mA cm −2 with a low Tafel slope of 80 mV dec −1 , and superior long-term stability toward HER. This work provides a new structural design to high-rise architectural structures for efficient catalytic application.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Guijuan Wei,Xixia Zhao,Kun Du,Zhaojie Wang,Ming Liu,Shuo Zhang,Shutao Wang,Jun Zhang,Changhua An
To date, zero-dimensional carbon quantum dots (CQDs), as a new carbon nanomaterials, have attracted attention in the improvement of the electrical conductivity for electrode materials. However, few attempts have been made to the use of CQDs as the structure-directing agent for the assembly of functional micro/nanoelectrodes. Herein, we have developed a general, and simple strategy to fabricate 3D porous hierarchical carbon quantum dots (CQDs)/M x O y (M = Co, Ni) composite nanostructures from thermolysis of corresponding CQDs/M(OH) y , where CQDs play crucial role as a structure-directing agent in tuning the morphologies of the M(OH) y . With the merits of the large electroactive surface area, superior electronic conductivity of CQDs, and fruitful porous structure, the as-fabricated battery-type electrode materials present amazing supercapacitor performance. For example, the as-made porous hierarchical CQDs/Co 3 O 4 nanoarchitectures exhibited remarkable electrochemical performance with 1603 F g −1 at 1 A g −1 , excellent rate capacity of 70.6% from 1 to 100 A g −1 , superior cycling ability (97.0% capacity remained after 2000 cycles). Furthermore, the CQDs/Co 3 O 4 //AC hybrid supercapacitor (HSC) exhibits a high specific capacity of 210.4 F g −1 with 74.8 W h kg −1 . The present work can be enlarged for the design of other functional 3D hierarchical micro-nanostructures in the fields of energy storage, catalysis, and photo/electrocatalysis.
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CATALYSIS TODAY
·
2024
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IF 5.2
Yushuai Sang,Mingze Yang,Hong Chen,Yongdan Li
Catalytic lignin solvolysis (CLS) holds promise for efficient lignin utilization, yielding small molecules with minimal or no char formation. However, the role of different active sites of catalyst in CLS are rarely discussed. Here, Ni catalysts on different supports, i.e., SiO 2 , Al 2 O 3 , MgO, and ZrO 2 , were prepared with the aim of manipulating the relative importance of metal and acid-base functionalities to investigate the role of different active sites in the enzymatic hydrolysis of lignin (EHL) ethanolysis. The main ether linkage, i.e., β-O-4, in EHL is cleaved without the participation of a catalyst. Metal sites suppress repolymerization through hydrogenating active intermediates, while acid and base sites facilitate the conversion of phenolic monomers into complex alkylated and etherified products and also promote repolymerization reactions. Among the catalysts, Ni/SiO 2 demonstrated the highest hydrogenation activity and yielded the most monomers (24.7 wt %) at 280 °C for 6 h under 2 MPa H 2 in ethanol. These findings shed light on the catalytic mechanisms in CLS, offering valuable insights for future catalyst design.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2024
·Vol. 107
·期 10
·6764-6773
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IF 3.5
Huihui Yan,Kun Wang,Liping Zhao,Peng Zhang,Han Chen,Jing Liu,Lian Gao
A new type of Ni/Al 2 O 3 self-supporting catalysts, with high specific surface area, was fabricated by blow-spinning technology. These Ni/Al 2 O 3 self-supporting catalysts are hollow flexible fibers and were utilized for the dry reforming of methane. The Ni/Al 2 O 3 catalysts exhibited exceptional catalytic performance, maintaining their activity for over 150-h at a high temperature of 800°C. The Ni nanoparticles disputed on the hollow fibers demonstrated remarkable resistance to sintering and coking during high-temperature catalysis. This was a noteworthy feature, as sintering and coking are common challenges faced by catalysts during high-temperature reactions. Furthermore, the catalysts retained its activity even after a rigorous 150-h test at 800°C, indicating its durability and stability. Importantly, the Ni/Al 2 O 3 self-supporting could be successfully reactivated after the test, further highlighting its reusable nature. This study offers promising new avenues for the development of high-temperature, self-supporting, and reactivatable catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Shaojun Sun,Chunyan Zhang,Mingxin Ran,Yujie Zheng,Chuanhua Li,Yu Jiang,Xuemin Yan
Developing efficient, stable, and cost-effective catalysts is crucial for hydrogen production through electrolysis of water. In this study, a comprehensive work was conducted on the electrocatalytic hydrogen and oxygen evolution performance of nickel-based phosphides doped with metallic iron. The Ni 5 P 4 /Ni 2 P/Fe 2 P catalysts with heterostructure were synthesized via a simple two-step synthetic route: (i) NaBH 4 pretreatment and in situ hydrolysis, (ii) low-temperature phosphating. It was found that iron doping not only improves the dispersibility but also increases the valence state of nickel in phosphating products. The Ni 5 P 4 /Ni 2 P/Fe 2 P-2 catalyst prepared with a molar ratio of 3 between Ni and Fe exhibits the best performance for HER and OER. In detail, only 185 and 190 mV overpotentials in acidic and alkaline electrolytes are required when the current density of hydrogen production is 10 mA cm −1 , respectively. To achieve the same current density under alkaline conditions, an overpotential of 215 mV is required for oxygen evolution, which is superior to IrO 2 . This work would enlighten the construction of more advanced bifunctional catalysts (HER and OER) via metal Fe doping.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
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IF 15.7
Mengran Liu,Canyu Liu,Tianfang Yang,Shixiang Hu,Siyun Li,Shizhe Liu,Yang Liu,Ye Chen,Bingcheng Ge,Shuyan Gao
Transition metal Ni anchored in carbon material represents outstanding 2e − oxygen reduction reaction (ORR) catalytic selectivity, but enhancing the adsorption strength of intermediate *OOH to promote its selectivity remains a major challenge. Herein, the NiX/Ni@NCHS composite catalyst with heteroatom doping (O,S) is modulated by controlling partial pyrolysis strategies on honeycomb-like porous carbon to manipulate the electronic structure of the metal Ni. With the synergistic effect of honeycomb structure and O atom, NiO/Ni@NCHS-700 exhibits an exceptional H 2 O 2 selectivity of above 89.1% across a wide potential range from 0.1 to 0.6 V in an alkaline electrolyte, and an unexpected H 2 O 2 production rate up to 1.47 mol g cat ‒1 h ‒1 @0.2 V, which outperforms most of the state-of-the-art catalyst. Meanwhile, NiS/Ni@NCHS exhibits excellent electrocatalytic performance, with 2e − ORR selectivity of 91.3%, H 2 O 2 yield of 1.85 @0.3 V. Density functional theory simulations and experiments results reveal that the heteroatom doping (O,S) method has been employed to regulate the adsorption strength of Ni atoms with *OOH, and combined with the self-sacrificing template-assisted pyrolysis approach to improve the microstructure of catalysts and optimize the active site. The heteroatom doping method in this work provides significant guidance for promoting 2e − ORR electrocatalysis to produce H 2 O 2 .
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Journal of Materials Chemistry A
·
2025
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IF 9.5
Qin Tang,Lingyue Wang,Shenglong Zhang,Pengfei Xue,Yuye Zhang,Hongbo Li,Dongdong Zhu
It is critical to develop highly efficient electrocatalysts for water splitting to achieve energy-saving hydrogen production. Recently, fullerene-based electrocatalysts have been widely reported for cathodic hydrogen evolution reaction (HER), while their application for intrinsically sluggish oxygen evolution reaction (OER) at the anode has been rarely explored. Herein, a novel OER electrocatalyst, NiFe-OC60, was prepared by introducing Ni and Fe species on fullerol C60(OH)x. Fullerene-based carbon support can provide a high surface area, and be served as an electron buffer due to its inherent electron-withdrawing property. Besides the synergistic effects between Ni and Fe, fullerene-based carbon support promotes the generation of high-valence Ni3+ species, thus contributing to improved OER performance. The as-synthesized NiFe-OC60 supported on glassy carbon electrode exhibits excellent OER results with a relatively small overpotential of 314 mV at the current density of 10 mA cm−2, and a small Tafel slope of 38.62 mV dec−1 in the alkaline solution. Our work demonstrates fullerene-based materials as promising electrocatalysts for emerging clean-energy related technologies.
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JOURNAL OF ETHNOPHARMACOLOGY
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2024
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IF 4.8
Yun Li,Teng-Teng Ren,Shan-Shan Liu,Ling Zhang,Hong Yi,Chun Li,Liang-Mian Chen,Hui-Min Gao,Li-Hua Yan,Xiao-Qian Liu,Zhi-Min Wang
Ethnopharmacological relevance Dang-Gui-Si-Ni (DGSN) decoction is a classic prescription in the clinical practice of traditional Chinese Medicine (TCM). DGSN decoction is often used to relieve symptoms of cold coagulation and blood stasis recorded by Treatise on Febrile Diseases ( Shang Han Lun ) and treat Raynaud's disease, dysmenorrhea, arthritis, migraine in TCM clinic. Accumulated evidences have suggested that this diseases are related to microcirculation disturbance. However, the anticoagulant activity and underlying mechanisms of DGSN decoction responsible for the therapeutic not well understood. Aim of the study The fingerprint and anticoagulant activity in vivo-in vitro of DGSN decoction were evaluated to strengthen the quality control and activity study of formulas. Materials and methods The chemical components of DGSN decoction were analyzed by HPLC and its fingerprint similarity were evaluated by “Chinese Medicine Chromatographic Fingerprint Similarity Evaluation Software (2012 Edition)". The anticoagulant activity of DGSN decoction was assessed by measuring four coagulation factors (PT, TT, APTT, FIB) in vitro . Zebrafish thrombosis model induced by punatinib was established to evaluate the activity of improving microvascular hemodynamics in vivo . Quantitative real-time polymerase chain reaction (q-PCR) were adopted to compare the changes in the RNA expression levels of coagulation factor II (FII), VII (FVII), IX (FIX) and X (FX) in zebrafish thrombosis model. Results The fingerprint similarity evaluation method of DGSN decoction was established. The results showed that 18 samples had higher similarity (S1–S18 > 0.878). Pharmacodynamic results showed that DGSN decoction could extend PT, TT and APTT, and reduce FIB content in vitro . Meanwhile, it markedly enhanced the cardiac output and blood flow velocity at low dosage (500 μg mL −1 ) in vivo . q-PCR data demonstrated that DGSN decoction (500 μg mL −1 ) could downregulate the RNA expression of FII, FVII, FIX and FX. Interestingly, there were a bidirectional regulation of FII, FIX and FX in a certain concentration range. In general, DGSN decoction can significantly improve hemodynamics and downregulate coagulation factors, and the results were consistent both in vitro - in vivo . Conclusion The fingerprint study provide a new perspective for improving the quality control of DGSN decoction. DGSN decoction possess anticoagulant activity by regulating multiple coagulation factors simultaneously. Thus, it has the potential to develop into the novel raw material of anticoagulant drugs.
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PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Bingyan Sun,Haifeng Xu,Tan Li,Wenjie Guan,Kaige Wang
Upcycling waste plastic into aromatics presents an attractive strategy to tackle both plastic pollution and energy challenges. However, previous studies often rely on high temperatures, precious metals, and have broad product distributions. In this study, we reported that a Ni/ZSM-5 bifunctional catalyst can directly convert polyethylene (PE) into methylated aromatics with high selectivity under mild conditions, while eliminating the requirement for hydrogen gas and solvents. The liquid yield could attain up to 70.3 %, and the aromatics yield could achieve up to 51.7 %. Over 78.4 % of the aromatics were methylated aromatics including toluene, xylene, and mesitylene. Polymer chains underwent dehydrogenation over Ni and the acid sites in ZSM-5, forming C C bonds. Certain of these bonds evolved into carbenium ions through the process of proton transfer at the acid sites. The optimization of Ni and acid sites enhanced the oligomerization, cyclization, and aromatization process. The extra mesopores created by Ni on the molecular sieve aid in the generation of aromatics. Furthermore, the Ni/ZSM-5 catalyst demonstrated the ability to convert typical commercial grades of PE plastic, such as gloves and bottles, into aromatics with a selectivity of up to 61.1 %. It offers an economically feasible and environmentally friendly upcycling avenue for the circular economy of plastics.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
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IF 4.1
Yeshuang Wang,Zhelin Su,Mingxian Duan,Huiling Fan,Ju Shangguan,Chao Yang
Metal oxides-based adsorbents used for desulfurization encounter significant challenges during practical application owing to their inferior reusability and the nature of solid waste of their desulfurization products. This situation might be alleviated to some extent through a rational design of Ni–Mo composite, enabling them firstly to be used as adsorbents for H 2 S removal, and then being utilized as catalysts after desulfurization for C 4 H 4 S hydrogenation. The Ni–Mo composites before and after desulfurization were characterized using XRD, FT-IR, SEM, N 2 adsorption–desorption, XPS, CO 2 -TPD and H 2 -TPR techniques. The experimental findings suggested that Ni and Mo species function as primary active sites for H 2 S adsorption and C 4 H 4 S hydrogenation reactions, respectively. The Ni and Mo composite greatly facilitated the coupling of these two reactions due to the formation of NiMoO 4 phase. This novel active phase not only boosted the interaction between metal and H 2 S but also promoted the formation of weak and moderate alkaline sites, thereby significantly enhancing desulfurization performance. Importantly, this active phase fostered the sulfurization of Mo species and transforming into a Ni–Mo–S component, further favoring the subsequent catalytic reaction in C 4 H 4 S hydrogenation. Consequently, the prepared Ni–Mo composite oxides exhibited excellent properties in H 2 S adsorption and C 4 H 4 S hydrogenation activity, surpassing the capabilities of single metal adsorbents and commercial hydrogenation catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jin Liu,Yao Wei,Ruitao Li,Yuxin Liu,Hailing Yu,Xuan Zhou,Bo Wu,Tiejun Lin,Liangshu Zhong
Direct conversion of methane to acetic acid with high activity and selectivity over non-noble metal-based catalysts under mild reaction conditions remains a grand challenge. Specifically, 1.2Ni-ZSM-5 with 88.9 % isolated Ni sites achieved a high acetic acid yield of 2920 μ mol/g cat. and a remarkable selectivity up to 82.3 % from methane oxidative carbonylation. Combined with high angle annular dark field scanning transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy analyses, it was revealed that the isolated Ni species with Ni-O 6 moieties anchored in the micropores of ZSM-5 were suggested to be the active sites. The isotopic labeling experiments and monitoring of reaction intermediates demonstrated that CH 3 COOH was formed via the direct coupling of methyl radicals and carbon monoxide molecules. This work suggests that the well-designed Ni sites can promote the transformation of CH 4 to C 2+ oxygenates instead of traditional C 1 oxygenates as main products.
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危险品化学品经营许可证（带存储）