CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Xue Zhang,Chunxia Wu,Ye Bu,Ying Liang,Zhitong Wang,Jing Li,Daoxiong Wu,Xinlong Tian,Peilin Deng
Exploring efficient and durable methanol oxidation reaction (MOR) electrocatalysts is crucial for the industrialization of direct methanol fuel cells. Herein, we designed MOR electrocatalyst of PtRu/Ni-N-C, in which PtRu nanoclusters (PtRu NCs) are loading on nitrogen-doping carbon support anchoring Ni single atoms (Ni-N-C). Compared with PtRu NCs and Pt/C, PtRu/Ni-N-C exhibits more excellent MOR activity with 2050 mA mg pt -1 and tougher anti-CO toxicity over 6000 s CA test, proving that the synergetic effect of nanoclusters and single atoms support enhance MOR activity and resistance to anti-CO toxicity. The fine spectroscopy analysis and density functional theory (DFT) calculations demonstrate that the strong metal-support interaction (SMSI) between nanoclusters and single atoms, facilitating the electron transfer of about 0.4 e from PtRu NCs to the Ni-N-C support, effectively reduces the d -band center of Pt to weaken the adsorption capacity of *CO and *COOH intermediates. Moreover, the synergistic sites derived PtRu NCs coupling Ni single atoms accelerate *OH adsorption, promoting the adjacent *CO removal. This work offers deep insight into the SMSI effect between nanoclusters and single atoms support to design the efficient Pt-based MOR electrocatalysts.
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ADVANCED MATERIALS
·
2026
·
IF 29.1
Jiage Yu,Wei Liu,Lu Bai,Benqiang Tian,Qingyi Zhu,Qianxi Yang,Linlin Zhou,Haoyang Wu,Yuan Wang,Boyuan Li,Xiangrong Jin,Yun Kuang,Jiazhan Li,Xiaoming Sun
CO 2 electroreduction typically requires large overpotentials to sustain high reaction rates, which at current densities approaching 1 A cm −2 inevitably intensify competition from the hydrogen evolution reaction (HER), making it difficult to simultaneously sustain high product selectivity (>95%). In this study, hollow Ni─NC (H-Ni-NC) was synthesized using nanoscale silica sphere templates and atomic Zn as a sacrificial pore-former within the carbon shell. The optimized H-Ni-NC achieves a current density of −1.0 A cm −2 with over 95% CO Faradaic efficiency in a flow cell. The high performance was attributed to the hollow sphere architecture enriched with gas-permeable through-pores. Notably, the Zn dosage selectively modulates the shell through-porosity, without altering hollow sphere macrostructure or the active-site structure, thereby enabling a systematic investigation of porosity effects. Finite-element simulations provide a qualitative framework suggesting a trade-off between reactant transport and active surface area with increasing porosity in hollow spherical catalysts. This work underscores that engineering of the nanoscale mass-transport environment surrounding active sites plays a critical role in designing high-efficiency electrocatalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Liquan Xiong,Ying Wang,Di Gao,Yueqi Song,Dongsheng Chen
Hydrogen energy is the core of future clean energy, and the study of hydrogen evolution reaction (HER) electrocatalytic mechanisms is essential for efficient production. The development of efficient and low-cost electrocatalysts is a key challenge in achieving ideal hydrogen generation. In this study, a Ni-BDC/TpPa-1 heterojunction material was prepared for the first time, which was converted into a derived heterojunction material (NiO@Ni/N-C) after high-temperature pyrolysis treatment, exhibiting excellent electrocatalytic activity in an alkaline solution. Without iR compensation, the overpotential of HER is only 83 mV at a current density of 10 mA·cm⁻². Compared with thermally decomposed Ni-BDC and TpPa-1 monomer, its electrocatalytic activity is improved by 158 and 435 mV, respectively, and it exhibits excellent stability over 100 h. The design of this novel material offers a new solution for enhancing the efficiency of transition-metal-based catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Manli Wang,Zhicheng Liu,Ming Hou,Xu Luo,Wenbin Yang,Hongjie Zhang,Xiaoming Song,Zhigang Shao
The irreversible degradation of platinum-based catalysts caused by strong sulfur dioxide (SO₂) adsorption poses a primary obstacle to the oxygen reduction reaction (ORR), limiting the practical application of proton exchange membrane fuel cells. Herein, we design and synthesize an anti-SO 2 poisoning Pt-based catalyst comprising Pt nanoparticles anchored on a single-atom Ni-N-HCNs support. The obtained catalyst (Pt/Ni-N-HCNs) exhibits exceptional tolerance to SO₂ poisoning, demonstrating a minimal negative shift of only 47.7 mV in the half-wave potential after contamination, compared to the 79.4 mV shift observed for commercial Pt/C. More importantly, Pt/Ni-N-HCNs catalyst demonstrates significantly enhanced ORR performance, with a mass activity of 0.58 A mg Pt −1 and a specific activity of 1.57 mA cm −2 , representing 1.2-fold and 2.7-fold improvements over commercial Pt/C, respectively. Density functional theory (DFT) calculations and XPS results reveal that the strong metal-support interaction (SMSI) induces the downshift of the d-band center of Pt, thereby weakening SO 2 adsorption and facilitating SO 2 removal. Furthermore, the Ni N site in Ni-N-HCNs support exhibits high activity for SO 2 oxidation, promoting the effective removal of SO 2 from adjacent Pt sites. Both effects synergistically enhance the resistance to SO 2 poisoning of the Pt/Ni-N-HCNs catalyst without sacrificing ORR performance. This work provides insights into the design of poison-resistant electrocatalysts and the development of energy conversion systems with high environmental applicability.
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ENERGY & FUELS
·
2025
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IF 5.3
Hui Yang,Libo Han,Haiquan Su,Lili Wan,Yue Su
Dry reforming of methane (DRM) reaction has attracted much attention due to its important implications for the environment and energy. The nonprecious metallic nickel is a promising active metal in DRM catalysts because of its low price and high activity. However, nickel-based catalysts are prone to deactivation due to sintering and carbon deposition, which is the main factor limiting the industrial application of the DRM reaction. Herein, a highly stable DRM catalyst has been developed, which was a highly dispersed nickel-based catalyst Ni/N-C-DS (Ni supported on N–C support prepared by the double-solvent (DS) method), prepared by impregnating Ni2+ into the cavities of ZIF-8 using the double-solvent method (DS), followed by a one-step carbonization process. The results showed that the Ni/N-C-DS catalyst exhibited smaller metallic Ni nanoparticles, more dispersed Ni species, and richer pore structures. At a reaction temperature of 800 °C, the Ni/N-C-DS catalyst exhibited satisfactory DRM catalytic activity and stability, with CH4 and CO2 conversion rates reaching 82 and 85%, respectively. The H2/CO ratio approached 1, and no deactivation was observed during 300 h of continuous operation. A thorough study of the catalyst’s structure–activity relationship revealed that the high dispersion of Ni0 in the Ni/N-C-DS catalyst was the main source of high activity for the DRM reaction, while the high stability in the later stage (80–300 h) of the DRM reaction was mainly attributed to the synergistic effect between the in situ reduced Ni0 and the initially highly dispersed Ni0.
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Catalysts
·
2022
·Vol. 12
·期 12
·1525
·
IF 4.501
Sai Che,Na Ta,Fan Yang,Yulong Yang,Yongfeng Li
Rational design and construction of cost–effective electrocatalysts for efficient hydrogen production has attracted extensive research attention worldwide. Herein, we report the construction of a transition metal selenide/carbon composite catalyst featuring uniform NiSe nanoparticles anchored to single Ni atom doped porous carbon structure (NiSe/Ni–N–C) via a facile one–pot pyrolysis of low–cost solid mixtures. NiSe/Ni–N–C exhibits remarkable catalytic performance towards hydrogen evolution reaction (HER) in 1.0 M KOH, requiring a low overpotential of 146 mV to reach a current density of 10 mA cm−2. The unique carbon layer encapsulation derived from the enwrapping of fluid catalytic cracking slurry further renders NiSe/Ni–N–C excellent for long–term durability in electrolyte corrosion and nanostructure aggregation. This work paves the way for the design and synthesis of highly efficient composite HER electrocatalysts.Keywords:NiSe nanoparticle;single atom catalyst;interfacial electronic engineering;hydrogen evolution reaction
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Chemistry-An Asian Journal
·
2024
·
IF 3.5
Yicheng Wang,Qiyu Zhang,Chenxu Wang,Ayeza,Yating Zhang,Chao Hu
The utilization of renewable energy for electrocatalytic carbon dioxide reduction reaction (CO 2 RR) represents a pivotal technology in sustainable carbon conversion. Single-atom catalysts (SACs) featuring transition metal-nitrogen-carbon (M−N−C) structures have demonstrated exceptional electrocatalytic efficacy in CO 2 RR by maximizing atom efficiency. Nevertheless, further investigation is warranted to optimize the catalytic performance of SACs through the selection of suitable carbon sources and supports, as well as the modulation of the microenvironment surrounding individual metal atoms. In this study, a sulfur-doped Ni−N−C catalyst was prepared using a two-step strategy involving metal ion adsorption and thermal decomposition, with porous ion exchange resin serving as the carbon source. Due to the uniform distribution of single atom active centers on the resin-based carbon support and sulfur doping, this catalyst efficiently converts CO 2 into CO with a Faradaic efficiency exceeding 90 % within the range of −0.69~−1.29 V (vs. RHE), reaching a maximum value of 97.7 % (−0.79 V vs. RHE). Theoretical calculations indicate that second-shell sulfur doping effectively promotes coupled transfer of protons and electrons, leading to a significant reduction in Gibbs free energy barriers for CO 2 RR intermediate products.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 35
·14970-14978
·
IF 3.288
Jingchuang Zhao,Yingzhen Zhang,Xianyu Kang,Yancai Li
Direct methanol fuel cells (DMFCs) have been extensively studied for developing a new non-precious metal catalyst to replace commercial platinum catalysts, due to their expensive cost and susceptibility to CO poisoning. In this work, nanocomposites of nickel oxide/nickel supported by N-doped carbon (NiO/Ni–N/C) were prepared by using a hydrothermal method and further carbonization at different temperatures. The surface morphology and composition of the NiO/Ni–N/C nanocomposites were characterized by using X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). As observed through electrochemical experiments, the NiO/Ni–N/C nanocomposite modified glassy carbon electrode (NiO/Ni–N/C/GCE) exhibits high electrocatalytic activity for the methanol oxidation reaction (MOR) in alkaline solution. Among the nanocomposites, NiO/Ni–N/C carbonized at 500 °C (NiO/Ni–N/C500) displays the highest mass activity (1043 mA mgNi−1) at 0.73 V (vs. Ag/AgCl), which is much higher than that of Ni(OH)2/N–C and NiO/Ni–N/C carbonized at other temperatures (400, 600, and 700 °C). In addition, the catalytic activity of NiO/Ni–N/C500 is 2.12 times that of the commercial Pt/C. NiO/Ni–N/C500/GCE also possesses fast kinetics, excellent stability and CO tolerance. Therefore, the NiO/Ni–N/C500 nanocomposites have great application potential as MOR catalysts.
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Reaction Chemistry & Engineering
·
2020
·Vol. 5
·期 5
·886-895
·
IF 3.441
Xing-Gang Si,Yun-Peng Zhao,Qing-Lu Song,Jing-Pei Cao,Rui-Yu Wang,Xian-Yong Wei
A highly efficient Ni/N–C catalyst was synthesized by facile pyrolysis of a Ni-containing metal–organic framework (Ni-MOF), and its catalytic hydrogenolysis performance towards C–O bonds in lignin was evaluated in detail using diphenyl ether (DPE) as a model compound. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analyses show that the flower-like nanosheets of the Ni-MOF shrink, forming a loose and ordered spherical structure during pyrolysis. Under the optimal conditions, DPE was completely converted and the selectivity to monomers (benzene, cyclohexanol and cyclohexane) reached 99.1%. During the catalytic hydrogenolysis conversion (CHC) of DPE, the direct cleavage of the Caromatic–O bond affording benzene and phenol is the major reaction pathway, and a low H2 pressure is crucial to increase the monomer selectivity. Furthermore, Ni/N–C-450 shows high hydrogenolysis activity for other lignin-derived aryl ethers, such as benzyl phenyl ether, dibenzyl ether, dinaphthalene ether, benzyl 2-naphthyl ether and 3-methoxyphenol.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhicheng Liu,Manli Wang,Ming Hou,Yun Zhao,Wenbin Yang,Yangkai Han,Zhigang Shao
In traditional CO 2 electrolysis systems, oxygen evolution reaction (OER) consumes 90 % of the electricity input, whereas the product of oxygen holds minimal value. Moreover, the use of different electrocatalysts for the anode and cathode remains a challenge due to high capital costs of the electrolysis system. Substituting the OER with thermodynamically advantageous value-added anodic reactions and developing bifunctional electrocatalysts are crucial for the advancement of CO 2 electrolysis. In this study, for the first time, we present an innovative CO 2 electrolysis system that integrates CO 2 electroreduction reaction (CO 2 RR) with SO 2 electrooxidation reaction (SO 2 OR) and employ Ni-N-C as the bifunctional electrocatalysts to produce CO and H 2 SO 4 simultaneously. Notably, the novel CO 2 electrolysis system can reduce the cell voltage by 1.05 V, resulting in nearly 50 % reduction in energy consumption. This is also the first attempt to use Ni-N-C to catalyze SO 2 OR, showing markedly superior performance compared to commercial 20 % Pt/C. In-situ ATR-SEIRAS and DFT calculations demonstrate that the NiN 4 sites in Ni-N-C catalysts augment the direct conversion of *SO 2 to *HSO 4 - , identified as the rate-determining step for the SO 2 OR. This work provides guidance for the design of novel CO 2 electrolysis systems, the construction of bifunctional electrocatalysts, as well as the mechanistic investigation of the SO 2 OR.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 4
·928-935
·
IF 4
Yidan Sun,Fang Liu,Xuerong Wang,Kangkang Lu,Xiaojing Liu,Yan Huang,Fengjiao Yu,Yuhui Chen
Efficient catalysts are highly desirable for the selective electrochemical CO2 reduction reaction (CO2RR). Ni single-atom catalysts are known as promising CO2RR catalysts, while Ni NPs are expected to catalyze the competing HER. In this work, we have modified the Ni NPs by encapsulating them into porous Ni–N–C nanosheets (Ni@Ni–N–C), to boost the synergy between Ni NPs and dispersed Ni–N species towards CO2RR. The CO faradaic efficiency (FECO) reached 96.4% at −0.9 V and retained over 90% in a wide potential window. More importantly, FECO values of over 94% have been obtained from −50 to −170 mA cm−2 with a peak FECO of 99% in a flow cell. Our work demonstrates that the surface modification of Ni NPs can inhibit the unexpected HER and activate the surface sites, offering a practical design strategy for CO2RR catalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Ping Zhang,Hao Chen,Lin Chen,Ying Xiong,Ziqi Sun,Haoyu Yang,Yingke Fu,Yaping Zhang,Ting Liao,Fei Li
Atomically dispersed catalytic metal sites anchored on N-doped carbon support catalysts (M-N-C) show great prospects for CO 2 electroreduction. Here, single-layer NiZn layered double hydroxides (NiZn-LDHs) was used as a sacrificial assistant to fabricate single-Ni atom anchored on ultrathin porous carbon catalyst. NiZn-LDHs were exfoliated to single-layer by polyhydroxy compounds which took as the carbon resource in Ni-N-C, and single layer NiZn LDHs taking as the Ni resource could avoid the agglomeration of Ni atoms during calcining. The CO Faradaic efficiency (FE CO ) of the synthesized Ni-N-C catalyst exceeded 90% at −0.6 to −1.0 V and a FE CO of 95.2% with a current density of 24 mA cm −2 at −0.9 V. This work not only provides a new method for preparing M-N-C catalysts, but also offers an effective and controllable strategy for large-scale production of high-performance single-atom catalysts.
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