JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Xianping Ye,Jian Wu,Fenghua Chen
Fabrication of low-cost, stable and highly efficient catalysts for clean energy and environmental control applications is an urgent task. In this work, we have successfully synthesized a multifunctional two-dimensional rare earth-based LaOCl@hcp-Ni heterostructure via a simple one-pot method. Here, the semiconductor LaOCl nanoparticles were well deposited on the metastable metal hcp-Ni, and the hexagonal close-packed structure of hcp-Ni matched the layered-structure LaOCl to form a highly active LaOCl@hcp-Ni Schottky catalyst. Furthermore, LaOCl@hcp-Ni were tested for Photoelectrochemical (PEC) oxygen evolution reaction (OER) in alkaline media and the photocatalytic (PC) degradation of Rhodamine B (RhB) in aqueous solution. LaOCl@hcp-Ni shows excellent PEC-OER catalytic activity and RhB degradation performance under artificial simulated sunlight. This enhancement of PEC and PC performance is due to the Schottky interface constructed by the coupling of hcp-Ni and LaOCl, which generates an interface electric field to effectively promote the transfer of photogenerated electrons from the semiconductor LaOCl to the metal hcp-Ni through the interface. Thus, energy band gap of LaOCl with oxygen defects is adjusted to the visible light region and their valence state of La is lowered, realizing high-efficiency visible light catalytic activity. Thus, it would be a potential rare earth-based Schottky catalyst, which can be used for the PEC oxygen evolution and the PC degradation of organic pollutants.
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 6
·3507-3516
·
IF 9.3
Xinqi Zheng,Bo Chen,Juwen Gu,Songbai Qiu,Xiaoping Wu,Qian Zhang,Tiejun Wang
Direct reconstruction of fermentation of ethanol in water with high water content to higher alcohols is a promising way to produce value-added fine chemicals and bio-fuels. In particular, aqueous ethanol reconstruction under near-ambient conditions is a milestone goal, but facing great challenges. Herein, the highly active and thermostable hexagonal-close-packed (hcp) Ni dominated hcp/fcc-Ni@C catalyst was fabricated via a facile surfactant-induced carbonization strategy for direct reconstruction of fermentation of ethanol solution to C4+ higher alcohols at near-ambient temperature (<100 °C). A superior performance of >99% higher alcohol selectivity with 17.6% ethanol conversion was achieved. DFT analysis revealed a low energy barrier of ethanol dehydrogenation (rate-determining step) over hcp-Ni, which is crucial for the ultra-low temperature ethanol reconstruction in water. The induction effect of the amide group in surfactant precursors is the key to the formation of hcp-Ni. This work provides new insight into producing bio-based higher alcohols from readily accessible aqueous fermentation of ethanol under mild reaction conditions, which is very promising for large-scale combined applications in industry.
研究领域:
生物化学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Wenqi Li,Yongli Shen,Linxiu Dai,Changhua An
Rational design of highly efficient catalysts for the dehydrogenation of ammonia borane (AB) to produce hydrogen is still challenging. The size and shape effects of catalysts on the performance have been well documented in the past decades. Nevertheless, there is still much space for study on the crystal structure-dependent catalytic performance. Herein, In2O3-supported hexagonal-close-packed (hcp) Ni (hcp-Ni/In2O3) has been prepared via impregnation of corresponding nanoparticles onto In2O3. The stronger electronic metal–support interaction in hcp-Ni/In2O3 than in fcc-Ni/In2O3 endows it with high capacity to activate AB molecules. It exhibits excellent hydrogen evolution activity from catalytic dehydrogenation of AB with a rate of 7.5 molH2 mol–1Ni min–1, which is 1.7 times that of the supported fcc sample. The systematic experiments and DFT calculations demonstrate that the hcp catalyst possesses stronger hydrophilicity and lower activation energy for the dissociation of H2O than the fcc counterpart. Moreover, the assistance with sonication enhances the process of mass and heat transfer and accelerates the reaction. This work provides a new way for the achievement of efficient metastable catalytic systems and promotes the construction of advanced devices toward various applications.
研究领域:
材料科学
·
催化
·
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.5
Chaoyue Zhang,Mingrui Wang,Xinyue Han,Zheng Shen,Hongying Zhuo,Tianyu Zhang,Xiaofeng Yang,Yanqiang Huang
Metastable hcp-Ni enables the synthesis of highly dispersed and stable Ni/Al 2 O 3 catalyst • Highly dispersed Ni/Al 2 O 3 catalyst delivers 75.7% CO 2 conversion and 100-h stability • Original hcp-Ni particles spontaneously transform into fcc-Ni clusters of ∼2.3 nm • Small Ni clusters promote CO 2 methanation via monodentate formate intermediate • Fcc-Ni precursors undergo severe sintering to ultra-large and less-active particles Ni-based catalysts are promising candidates for CO 2 methanation while their practical applications are limited by particle agglomeration and deactivation. Here, we report a facile strategy to fabricate a highly dispersed and stable Ni/Al 2 O 3 catalyst using metastable hexagonal close-packed (hcp)-Ni as a precursor. Comprehensive characterization reveals that the initial hcp-Ni (∼12.0 nm) spontaneously transforms into uniform face-centered cubic (fcc)-Ni nanoparticles (NPs) of ∼2.3 nm on γ -Al 2 O 3 support during H 2 reduction and CO 2 methanation reaction. The small Ni particles contribute to improved Ni 0 proportion on catalyst surface. In contrast, the original fcc-Ni precursors are prone to sintering, forming ultra-large and less-active Ni aggregates. The highly dispersed Ni NPs derived from hcp-Ni enhance CO 2 adsorption-activation and facilitate the formate-mediated reaction pathway. The resulting hcp-Ni/Al 2 O 3 catalyst delivers a CO 2 conversion of 58.2% with a CH 4 selectivity of 85.4% at 460 °C and endows robust stability exceeding 100 hours. The optimal CH 4 space time yield reaches 179.5 mmol·g cat −1 ·h −1 , exceeding 2.4 times that of fcc-Ni/Al 2 O 3 . This work establishes a reliable synthesis paradigm rooted in crystal-phase regulation, enabling the manufacture of highly dispersed and stable Ni-based catalysts for efficient CO 2 methanation. Manufacturing Highly Dispersed and Stable Ni/Al 2 O 3 Catalysts from hcp-Ni for Enhanced CO 2 Methanation Download: Download high-res image (221KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Wenxiu Yan,Yongli Shen,Chao An,Lina Li,Rui Si,Changhua An
Tuning the crystal phase of metals and constructing the metal-oxide interface provide a new way to improve oxygen evolution reaction (OER) kinetics. Herein, we developed a room-temperature plasma topology conversion of Fe 3+ doping Ni(OH) 2 nanosheets to porous hcp Ni engineered by FeOx clusters. X-ray absorption fine spectra established that they were formed via Ni-O-Fe bonds. The metal oxide-metal interfaces with benign geometry and electronic structures enable it to be applied as efficient electrocatalyst, exhibiting overpotential of 226 mV at 10 mA cm −2 . In situ Raman spectra show that the interfacial action of FeOx cluster with Ni can stimulate the generation of active intermediate of γ-NiOOH, effectively promoting OER rate. DFT calculation further demonstrates the interaction accelerates desorption of O 2 molecules on the surfaces. This work provides a simple and robust strategy to synthesize oxide clusters engineering metastable metal nanocatalysts, offering new platform to explore efficient catalysts in various fields.
研究领域:
材料科学
·
电化学
✓ 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）