JOURNAL OF CATALYSIS
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2026
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IF 6
Yun-Jie Li,Dong Wang,Bi-Xi Wang,Zhen-Yi Du,Wen-Ying Li
Eliminated Ni particle size effects to isolate intrinsic SMSI effects. • Decoupled the roles of Ni sites and interfacial Ni-O v -Ti 3+ sites. • Exposed Ni sites serve as the primary sites for H 2 activation and hydrogenation. • Interfacial Ni-O v -Ti 3+ sites promote oxygenated intermediate deoxygenation. • Balancing Ni encapsulation and oxygen vacancies maximizes HDO activity. Efficient hydrodeoxygenation is essential for upgrading biomass- and coal-derived oils into high-quality fuels. Although strong metal–support interactions (SMSI) have been employed to promote hydrodeoxygenation, how SMSI-induced metal encapsulation and oxygen vacancy generation individually and collectively govern hydrodeoxygenation remains unclear. To eliminate the confounding influence of Ni particle size, a series of Ni@TiO 2− x catalysts with uniform Ni particle sizes but tunable SMSI strengths were engineered through tailored pretreatment strategies. Using a remarkably simple kinetic strategy, the mixed roles of Ni sites and oxygen vacancies were successfully decoupled, proving that Ni encapsulation inhibits hydrogenation while oxygen vacancies drive deoxygenation. Consequently, the catalyst with intermediate SMSI strength strikes an optimal balance by maximizing the density of oxygen vacancies while mitigating excessive metal encapsulation, thereby delivering the highest hydrodeoxygenation activity. Density functional theory calculations further demonstrate that interfacial Ni-O v -Ti 3+ sites enhance the adsorption of oxygenated intermediates and markedly lower the C–O bond activation barrier. The cooperative interplay between exposed metallic Ni sites and interfacial Ni-O v -Ti 3+ sites orchestrates H 2 activation and C–O bond cleavage, thereby enabling efficient hydrodeoxygenation and providing a design principle for SMSI-regulated interfacial catalytic systems. Download: Download high-res image (159KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
HuangJingWei Li,Chao Cai,Qiyou Wang,Shanyong Chen,Junwei Fu,Bao Liu,Qingnan Hu,Kangman Hu,Hongmei Li,Junhua Hu,Qiming Liu,Shaowei Chen,Min Liu
Hydrogen production by alkaline water electrolysis represents an effective route for low-cost and clean energy conversion. However, as hydrogen ions (H + ) are the minority species in alkaline media, the kinetics of hydrogen evolution reaction (HER) is markedly reduced. Concurrently, the transport of hydroxide ions (OH – ) is limited under large current density in alkaline oxygen evolution reaction (OER). Herein, Ni nanoparticles-decorated Mo-Ni microrods (Ni/Mo-Ni) are adopted to boost the ion adsorption . Finite-element simulations suggest that a strong local electric field around the Ni nanoparticles exponentially increases ion adsorption towards the electrode surface, which facilitates reaction kinetics and mass transfer for HER at the cathode and OER at the anode. Thus, the Ni/Mo-Ni electrode exhibits a low overpotential of only −24 mV for HER and + 215 mV for OER to reach the current density of 10 mA cm −2 , and can achieve an industrial alkaline splitting current density of 100 mA cm −2 at a low voltage of 1.76 V and stably operate for 87 h. This work suggests a new paradigm in the design and engineering of high-performance catalysts for alkaline electrolyzers.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2020
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IF 7.864
Ruiyang Zhang,Tao Ran,Yuehan Cao,Qian Zhang,Fan Dong,Guidong Yang,Ying Zhou
Catalysis oxidization has been known to be an effective technique in environmental remediation. However, low efficiency for oxygen activation and difficult recovery of the catalysts in powdery form significantly limit the practical application. In this work, a new-type monolithic α-Ni(OH)2/Ni-foam was fabricated by the hydrothermal process. We found that H atoms of α-Ni(OH)2 can significantly promote oxygen activation, which endows it with favorable NO and NO2 oxidization confirmed by theoretical calculation and in situ DRIFTS. Furthermore, the introduction of Ni foam accelerated the pollutant gas transfer and charge carriers’ separation because of its abundant porous structure and high conductivity and its monolithic property simplified the recycling operation. Consequently, the obtained α-Ni(OH)2/Ni-foam achieved an excellent NO oxidation (69.0%) and no toxic NO2 was detected under visible light illumination (λ > 420 nm), indicating its highly promising potential in environmental remediation. Our work provides a conceptually different fresh perception to promote oxygen activation for highly efficient gas purification.
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JOURNAL OF POWER SOURCES
·
2019
·
IF 7.467
Dandan Li,Genyan Hao,Wenjun Guo,Guang Liu,Jinping Li,Qiang Zhao
Novel nickel nanotube arrays (NTAs) on foamed nickel (NF) are developed by a facile electrochemical dealloying method to achieve a high hydrogen evolution reaction . Meanwhile, three dimensional heterostructure NiFe layered-double-hydroxide (LDH)@Ni NTAs electrode materials with strong interfacial interaction are prepared on NF by coupling ultrathin NiFe LDHs with Ni NTAs by electrochemical deposition , which demonstrate an excellent catalytic performance for oxygen evolution compared with NiFe LDH. Ni NTAs/NF require an overpotential of 101 mV to force the current density of 10 mA cm −2 for hydrogen evolution reaction because of the unique NTAs structure and the active sites for water dissociation provided by Ni 2+ on the Ni NTAs surface. NiFe LDH@Ni NTAs/NF exhibit a low overpotential of 191 mV at a current density of 10 mA cm −2 for oxygen evolution reaction due to the reliable electron transfer from the intermediate metallic Ni NTAs to the external the NiFe LDH layer and more active sites that are exposed by highly dispersed ultrathin NiFe LDH nanosheets . The development of self-supporting NiFe LDH@Ni NTAs and Ni NTAs electrodes for efficient overall water splitting in an integrated alkaline electrolyzer is achieved a current density of 10 mA cm −2 at 1.51 V, accompanying excellent long-term durability.
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ENERGY & FUELS
·
2019
·
IF 3.021
Jingwei Li,Lijuan Jiang,Shuai He,Licheng Wei,Rongfu Zhou,Jinming Zhang,Dingsheng Yuan,San Ping Jiang
Development of efficient, stable, and robust bifunctional electrodes is important for the practical and industrial application of water electrolysis technologies for renewable hydrogen production. Here, we report the fabrication of heterostructured Ni(OH)2 nanosheets/Ni3S2 nanoneedles grown on Ni foam, Ni(OH)2/Ni3S2/NF, as a highly active and mechanically strong bifunctional electrode for overall water splitting. The results indicate that heterostructured Ni(OH)2/Ni3S2 interfaces are the reactive center for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). The redistribution of electrons and formation of the Niδ+ and Sδ− active species serve as the hydroxyl and proton acceptors and significantly promote the transformation of intermediate species and charge transfer processes in both the OER and HER. The Ni(OH)2/Ni3S2/NF electrode shows overpotentials as low as 252, 279, and 319 mV to reach 30, 50, and 100 mA cm–2, respectively, for OER and 48, 79, and 185 mV to achieve 10, 20, and 100 mA cm–2, respectively, for HER in 1.0 M KOH solution. An alkaline electrolyzer assembled by bifunctional Ni(OH)2/Ni3S2/NF electrodes displays cell voltages of 1.80 V to deliver 100 mA cm–2 and is stable for over 100 h. This study demonstrates promising potential of the Ni(OH)2/Ni3S2/NF bifunctional electrode for advancing water-splitting technologies.
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ChemSusChem
·
2023
·
IF 8.4
Jiaji Zhang,Gaobo Lin,Jie Zhu,Sifan Wang,Wenhua Zhou,Xiangzhou Lv,Bolong Li,Jianghao Wang,Xiuyang Lu,Jie Fu
Graphical We find that the N-doped Ni particles can enhance the adsorption of CO 2 and modulate the configuration of adsorbed CO on Ni-N-C sites. As a result, the optimal catalyst can efficiently convert CO 2 into CO with a faradaic efficiency of 96.7 % and a current density of 500 mA cm −2 in a strongly acidic electrolyte. Electro-chemically reducing CO 2 in a highly acidic medium is promising for addressing the issue of carbonate accumulation. However, the hydrogen evolution reaction (HER) typically dominates the acidic CO 2 reduction. Herein, we construct an efficient electro-catalyst for CO formation based on a core-shell structure, where nitrogen-doped Ni nanoparticles coexist with nitrogen-coordinated Ni single atoms. The optimal catalyst demonstrates a significantly improved CO faradaic efficiency (FE) of 96.7 % in the acidic electrolyte (pH=1) at an industrial-scale current density of 500 mA cm −2 . Notably, the optimal catalyst maintains a high FE of CO exceeding 90 % (current density=500 mA cm −2 ) in the electrolyte with a wide pH range from 0.67 to 14. In-situ spectroscopic characterization and density functional theory calculations show that the local electron density of Ni-N-C sites is enhanced by N-doped Ni particles, which facilitates the formation of *COOH intermediate and the adsorption of *CO. This study demonstrates the potential of a hybrid metal/Ni-N-C interface in boosting acidic CO 2 electro-reduction.
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CHEMOSPHERE
·
2023
·
IF 8.8
Jiaming Zhang,Chao Yu,Longqian Xu,Zhenyu Zhao,Deli Wu
Electro-enhanced metal-free boron/peroxymonosulfate (B/PMS) system has demonstrated potential for efficient metal-organic complexes degradation in an eco-friendly way. However, the efficiency and durability of the boron activator are limited by associated passivation effect. Additionally, the lack of suitable methods utilizing in-situ recovery of metal ions liberated from decomplexation causes huge resource waste. In this study, B/PMS coupled with a customized flow electrolysis membrane (FEM) system is proposed to address above challenges with Ni-EDTA used as the model contaminant. Electrolysis is confirmed to remarkably promote the activation performance of boron towards PMS to efficiently generate • OH which dominated Ni-EDTA decomplexation in the anode chamber. It is revealed that the acidification near the anode electrode improves the stability of boron by inhibiting passivation layer growth. Under optimal parameters (10 mM PMS, 0.5 g/L boron, initial pH = 2.3, current density = 68.87 A/m 2 ), 91.8% of Ni-EDTA could be degraded in 40 min, with a k obs of 6.25 × 10 −2 min −1 . As the decomplexation proceeds, nickel ions are recovered in the cathode chamber with little interference from the concentration of co-existing cations. These findings provide a promising and sustainable strategy for simultaneous metal-organic complexes removal and metal resources recovery.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Zongpeng Zou,Tao Zhang,Li Lv,Wenxiang Tang,Guoquan Zhang,Raju Kumar Gupta,Yan Wang,Shengwei Tang
Dry reforming of methane (DRM) presents a sustainable approach to convert greenhouse gases CO2 and CH4 into syngas. However, the industrialization of DRM is hindered by the short catalyst lifespan due to carbon deposition. Carbon deposition on Ni-catalysts is attributed to Ni step edges, which serve as carbon nucleation centers. We propose an innovative strategy to prevent carbon nucleation by modulating Ni size to eliminate Ni step edges. Ni was loaded on MCM-41, SBA-15, and DFNS (dendritic fibrous nanosilica) to prepare three distinct Ni catalysts. By altering the precursor concentration using the proposed microemulsion antisolvent coprecipitation method, we successfully adjusted the Ni size on DFNS. Ni particles with a diameter of ∼5 nm were obtained on DFNS, exhibiting excellent Ni dispersion and a physical spacing effect due to the specific preparation method and porous structure. Carbon deposition rates on Ni/MCM-41 and Ni/SBA-15 were 30.23 mgc·gcat·–1·h–1 and 16.33 mgc·gcat·–1·h–1, respectively. Remarkably, the carbon deposition rate on Ni/DFNS was only 0.15 mgc·gcat·–1·h–1. The gasification rate of deposited C to CO on the 5 nm Ni particles loaded on Ni/DFNS was five times that of the polyhedral Ni particles of Ni/MCM-41. This was attributed to the elimination of Ni step edges, which weakened C adsorption strength and enhanced the reaction of deposited C with O* to form CO. Our proposed catalyst preparation strategy is based on designing the catalyst microstructure to eliminate carbon nucleation sites. This research provides guidance for designing or preparing Ni-based catalysts for DRM with reduced carbon deposition.
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ChemCatChem
·
2018
·Vol. 10
·期 20
·4689-4698
·
IF 4.674
Yan Liu,Ye Wu,Zarina Akhtamberdinova,Xiaoping Chen,Guodong Jiang,Dong Liu
Graphical High fives ! The catalyst 5Ni-5Ce exhibits the best catalytic performance in the dry reforming of shale gas and CO 2 . The introduction of Ce creates strong interaction between Ni and Ce, which enhances the electron transfer between them. And the substitution of Ni for Ce produces oxygen vacancies and defects, which can accelerate the adsorption and activation of the reactant gases molecule, further promoting the reaction. The dry reforming of shale gas (methane and ethane with an average ratio of 4 : 1) with carbon dioxide (DRS) is considered to be a promising way to produce syngas, which widens the utilization of shale gas and mitigates carbon dioxide emission. In this paper, Ce modified Ni-based catalysts were developed and the corresponding catalytic performances for DRS were investigated with a fixed bed reactor. Results showed that the catalyst containing 5 wt% of Ni and 5 wt% of Ce performed a best catalytic effect, including the selectivity of syngas and the carbon resistance performance, which is due to the good metal dispersion, strong interaction between Ni and Ce, and the formation of Ni-CeO x solid solution. The electron transfer between Ni and Ce, substitution of Ni for Ce, and the sequential oxygen vacancies or defects, play significant roles in activating CH 4 , C 2 H 6 and CO 2 . The conversion of reactant gas increased with temperature, while the selectivity of syngas is little affected with temperature. In addition, the desired catalyst containing 5 wt% of Ni and 5 wt% of Ce showed good stability in the long-time operation, which indicates that the Ce modified Ni-based catalyst is a promising one for the dry reforming of shale gas.
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ACS Catalysis
·
2019
·
IF 12.221
Xiaoqiang Zhang,Peifang Yan,Bin Zhao,Kairui Liu,Mayfair C. Kung,Harold H. Kung,Shanyong Chen,Z. Conrad Zhang
The catalytic properties of physical mixtures of Ni particles (100–200 nm) with nanoparticles of anatase TiO2 (TiO2-A), ZrO2, Al2O3, rutile TiO2 (TiO2-R), and CeO2 were investigated for the hydrodeoxygenation (HDO) of guaiacol. High selectivities to phenolics were obtained only for Ni mixed with anatase TiO2 (Ni and TiO2-A), while saturated hydrocarbons were the main products for the mixtures with other supports. By thermal treatment in hydrogen gas only at 300 °C or higher and subsequently separating the large Ni particles from the TiO2-A particles with a magnet, it was further discovered that there was migration of TiO2 from TiO2-A onto the large Ni particles, resulting in an amorphous TiO2 overlayer on the Ni particles as evidenced by high-resolution TEM, and vice versa, migration of Ni onto TiO2-A. The TiO2 overlayer rendered the Ni particles completely inactive as a hydrogenation/hydrodeoxygenation catalyst. Conversely, the small amounts of Ni (<1.5 wt %) migrated onto TiO2-A formed highly dispersed Ni, undetectable by high-resolution TEM (<2 nm), that were remarkably highly active for HDO of guaiacol, producing selectively phenolics. Such highly selective HDO catalysts could also be formed by incipient wetness impregnation of Ni in loadings above 2 wt % onto the TiO2-A, but it was essential to pretreat the sample in H2 at 300 °C or higher. Pretreatment in H2 at 200 °C generated catalysts that produced saturated ring products. The activity of the impregnated catalysts, as measured by guaiacol conversion, increased linearly with Ni loading below 0.5 wt %. The activity continued to increase with Ni loading but more slowly up to 2 wt %, beyond which there was little further change. The results suggested that two types of Ni species existed on the TiO2-A surface. One type consisted of a cluster of Ni atoms that were dominant on larger Ni particles that were active in aromatic ring hydrogenation and hydrodeoxygenation. They were readily covered by reducible TiO2-A at 300 °C or higher due to the traditional strong metal support interaction (SMSI) effect and became inactive. Another type was clusters of a very small number of Ni atoms, perhaps one atom, that were present as highly dispersed Ni clusters interacting strongly with the defect sites of TiO2-A. The strong interaction of this type of Ni with the TiO2 defect deterred TiOx migration allowing surface exposed Ni atoms to catalyze the HDO of guaiacol with very high selectivities that were not characteristic of typical Ni particles.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yuzhu Xue,Weinan Wang,Yanhong Zhang,Qinhua Fan,Ying Zhang,Chen Ling,Yuwei Pan
This study proposes a green purification strategy in which mild decomplexation of Ni-EDTA into other Ni complexes facilitates the efficient removal and recovery of nickel through resin adsorption. Decomplexation of Ni-EDTA by boron/Fe 2+ /H 2 O 2 (B/Fe 2+ /H 2 O 2 ) followed by resins adsorption was conducted for Ni(II) removal in Ni-EDTA. The Ni(II) removal efficiency could only achieve 1.3 % and 6.2 % while Ni(II) coexisted with EDTA but more than 10 times of higher when Ni(II) coexisted with EDTA-relatives via the single adsorption of commercial heavy metal-affined resins (D001 and D463), which attributed to the increased binding energies of these Ni-EDTA’s degradation products complexes than Ni-EDTA based on density functional theory (DFT) calculation. In comparing to precipitation, the resin adsorption required much less mineralization of EDTA to have a better removal efficiency of Ni(II). B improved the efficiency of Ni-EDTA decompexation by accelerating the recycle of Fe 3+ /Fe 2+ . The EDTA (and TOC) removal enhanced from 48.7 % (4.7 %) to 94.7 % (11.9 %) by B/Fe 2+ /H 2 O 2 process comparing to Fe 2+ /H 2 O 2 process. With the high EDTA but low TOC removal efficiency after B/Fe 2+ /H 2 O 2 treatment, Ni(II) removal efficiency via resins adsorption could maximum achieve 80.5 %, 2–3 times of that via regular precipitation method. In addition, B and resins exhibited good reusability in five cycles, and B/Fe 2+ /H 2 O 2 -resins process had excellent adaptability to different heavy metal complexes. B/Fe 2+ /H 2 O 2 -D463 system not only could reduce 78.4 % reagents cost compared with that of Fe 2+ /H 2 O 2 -precipitation process, but also could save much cost than other processes. The results provide new insights for the cost-effective treatment of EDTA-complexed heavy metal wastewater.
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RSC Advances
·
2024
·Vol. 14
·期 52
·39061-39068
·
IF 3.9
Han Xiao,Jiaming Dong,Yimin Zhang,Xiaohua Cao,Yanhong Li,Dedong He,Yongming Luo,Pingyan Wang,Hao Wang
The presence of abundant hydroxyl groups on the surface of Al2O3 can promote the dispersion of Ni species but produce an inactive NiAl2O4 phase at high temperatures. Moreover, the catalysts prepared by the conventional incipient wetness impregnation method lack the sites for the activation of CO2, which leads to coke deposition and thus affects the catalyst activity. The above restricts the utilization of Ni in conventional Ni/Al2O3 catalysts. In this paper, Al2O3 support was pre-treated by acetic acid to selectively remove hydroxyl groups without affecting the coordination environment of Al. Results revealed that the Al2O3 support after hydroxyl removal not only showed moderate metal–support interaction but also produced more sites for the adsorption and activation of the reactant, which significantly improves the utilization of nickel species and the stability of the catalyst. The conversion of CH4 and CO2 at 700 °C was as high as 88% and 90%, respectively, and has an excellent stability of 50 h. This study provides a feasible strategy for the design of highly active methane dry-reforming catalysts.
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