JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Long Liu,Siyuan Zhao,Yue Ji,Ziliang Wang
Photocatalysis, as a technology for splitting water to produce hydrogen, has been paid more and more attention. However, the catalyst has fewer active sites and a fast carrier recombination rate resulting in lower activity. In this work, BiOBr-Ni with Ni single atoms and oxygen vacancies was prepared by the microwave - assisted method. The SEM results show that the BiOBr-Ni surface layer is composed of nano-sheets. Electron paramagnetic resonance (EPR) indicates that the prepared BiOBr-Ni contains oxygen vacancies. XRD, XPS and spherical electron microscopy have proved that Ni exists in the form of single atom. In the process of photocatalytic hydrogen production, BiOBr-Ni showed excellent photocatalytic activity. DFT and experimental tests show that the improved photocatalytic hydrogen production is the joint action of oxygen vacancy and Ni single atom, which not only enhances the carrier separation efficiency but also greatly reduces the reaction energy barrier.
研究领域:
材料科学
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能源化学
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Haoquan Guo,Jiwu Zhao,Yu Chen,Xinyu Lu,Yue Yang,Chenrong Ding,Lizhi Wu,Li Tan,Jinlin Long,Guohui Yang,Yu Tang,Noritatsu Tsubaki,Xiaoli Gu
Lignin derivatives are one class of attractive alternative feedstocks for the production of renewable biofuels. Herein, hydrodeoxygenation (HDO) of lignin derivatives was carried out using a single-atom catalyst (SAC) comprised of Ni1 SAC on β-Mo2C. A number of lignin-derived compounds have been investigated, and nearly 100% yield of biofuel molecules was converted from various lignin derivatives through the HDO reaction, demonstrating that Ni1/β-Mo2C has remarkable potential for the production biofuels through catalytic hydrodeoxygenation of lignin derivatives. The reaction mechanism of DHE over single-atom catalyst Ni1/β-Mo2C was confirmed based on comprehensive characterizations of catalysts and DFT calculations. Interestingly, the Ni single-atom active sites alter the reaction pathway by shifting the geometry of the adsorbed intermediate from a vertical to horizontal conformation, which lowered the reaction energy barrier and improved the selectivity to biofuel molecules, resulting in extraordinary catalytic activity. This study suggests an avenue for single-atom catalysis in chemical transformations of lignin derivatives into biofuels.
研究领域:
化学工程
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催化科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Meng Liu,Caixia Miao,Yumeng Fo,Wenxuan Wang,Yao Ning,Shengqi Chu,Weiyu Song,Ying Zhang,Jian Liu,Zhijie Wu,Wenhao Luo
Precisely tailoring metal single-atoms within zeolite scattfolds and understanding the origin of the unique behavior of such atomically dispersed catalysts are pivotal and challenge in chemistry and catalysis. Herein, we have successfully fabricated Ni single-atoms within BEA zeolite (Ni 1 @Beta) through a facile in situ two-step hydrothermal strategy, notably without using any chelating agent for stabilizing Ni species. With the aid of advanced characterization techniques, such as aberration-corrected high-angle annular dark-field scanning transmission electron microscopy, X-ray absorption spectroscopy, etc., and combined with density functional theory calculations, the nature and micro-environment of isolated Ni species, which are incorporated within 6-membered rings and stabilized by four skeletal oxygens of Beta zeolite, have been identified. The as-obtained Ni 1 @Beta exhibits a superior performance in terms of activity (with a turnover frequency value up to 114.1 h –1 ) and stability (for 5 consecutive runs) in the selective hydrogenation of furfural, surpassing those of Ni nanoparticle analogues and previously reported Ni-based heterogeneous catalysts. This study provides an efficient strategy for the fabrication of non-noble metal single-atoms within zeolites, which could be of great help for the design of metal-zeolite combinations in the chemoselective reactions involved in biomass conversion and beyond.
研究领域:
催化化学
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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
FUEL
·
2022
·
IF 8.035
Ming Jiang,Xiaopeng Chen,Linlin Wang,Jiezhen Liang,Xiaojie Wei,Weijian Nong
Lignin is the most abundant renewable aromatic resource in nature; thus, the development of an efficient and economical catalysts that can depolymerize lignin into value-added aromatic monomers is highly desirable. Here, we report a single-atom Ni catalyst ( x Ni/CeO 2 -S, where x represents the Ni loading), in which the single-atom Ni sites are anchored to the oxygen vacancies on CeO 2 nanospheres, for the conversion of cellulolytic enzyme lignin (CEL) via depolymerization and hydrodeoxygenation. The 1.0Ni/CeO 2 -S catalyst performed the best, achieving a lignin oil (LO) and maximum monomer yield of 84.3 wt% and 32.6 wt%, respectively; a higher heat value of 31.64 MJ/Kg is achieved for LO compared to 23.03 MJ/Kg for CEL. Thus, single-atom nickel catalyst exhibited excellent activity and stability in promoting the depolymerization of lignin. These results validate the viability of single-atom metal catalysts for the conversion of lignin resources.
研究领域:
催化化学
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可再生资源利用
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Huan Wang,Shu-Wei Yin,Jianchuan Liu,Weitao Wang,Zhen-Hong He,Kuan Wang,Zhi-Hao Zhao,Zhao-Tie Liu
Ni, especially Ni single atom catalysts (SACs) are the most promising electrocatalyst in the reduction of CO 2 to CO. However, the high energy barrier for the formation of *COOH on Ni SA sites leads to a high overpotential for CO 2 RR, which severely hinders the CO production efficiency. How the coupling effect of Ni SAs and Ni nanoparticles (NPs) sites improve the performance of Ni-based electrocatalysts is interesting to be investigated. Herein, theoretical calculations revealed that the synergy of Ni SAs and Ni NPs could efficiently lower the energy barrier of the *COOH formation via promoting the H 2 O dissociation process to accelerate the *H supply for CO 2 protonation as well as promote the CO 2 adsorption and CO desorption, thus improving catalytic activity. Based on the theoretical study, Ni-N 4 SA coupled with Ni nanoparticles supported on nitrogen-doped carbon nanotubes (Ni-N 4 Ni NP /NCNT) was designed. As electrocatalyst, the Ni-N 4 Ni NP /NCNT showed an ultralow onset overpotential of 60 mV for CO 2 RR-to-CO, and achieves a FE CO of ∼99 % from an overpotential of as low as 160 mV, outperforming state-of-the-art Ni SACs. This work not only sheds new light for the rational synthesis of Ni-based catalysts with both Ni SAs and Ni NPs sites to achieve efficient CO 2 RR to CO, but also offers an in-depth insight for the origin of efficient performance of cooperative Ni SA -Ni NP catalysts.
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
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 10
·e18161
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IF 3.7
Zhanshuai Ma,Tianyu Zhang,Lili Lin,Aijuan Han,Junfeng Liu
Developing highly active, selective, and stable electrocatalysts for the CO 2 reduction reaction (CO 2 RR) is essential to relieve the greenhouse effect and the energy crisis. Traditional catalytic electrodes require ionomer binders, which inevitably impose undesired high CO 2 transport resistance and block the active sites. Herein, Ni single atoms anchored on nitrogen-doped carbon nanoarrays (denoted as Ni-SAC-NA) were developed as the electrode without additional ionomers for efficient CO 2 RR. The unique nanoarray structure provided a higher specific surface area, more exposed active sites, and enhanced electron/mass transport due to its short diffusion pathway and ionomer-free nature. As a result, the Ni-SAC-NA electrode exhibited enhanced activity of CO 2 RR and selectivity towards CO with Faradaic efficiency of 96.7%, turnover frequency of 27,504 h −1 , and cathodic energy efficiencies of 54.9% at −0.88 V (vs. RHE). Our findings provide a rational design strategy for CO 2 RR electrocatalysts by constructing ionomer-free electrodes.
研究领域:
材料科学
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能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Conghan Zhang,Jiating Cheng,Fan Yang,Yang Sun,Xinyang Sun,Kexin Wei,Guang Ma,Junpu An,Meitong Zhao,Jiahui Liu,Yongfeng Li
Electrolytic water splitting using transition metal sulfide catalysts has garnered a lot of attention lately. Herein, a composite material consisting of Mo-doped Ni 3 S 2 nanoparticles supported on N-doped carbon layers with anchored Ni single atoms (Mo–Ni 3 S 2 /Ni–N–C) was synthesized using a two-step hydrothermal process. These features enable Mo–Ni 3 S 2 /Ni–N–C to achieve low overpotentials of 71, 58, and 89 mV for the hydrogen evolution reaction (HER) at 10 mA cm −2 in 1 M KOH, 0.5 M H 2 SO 4 , and 1 M PBS, respectively. After 20 h of durability testing, its current density retains over 95 % of the initial value across diverse pH electrolytes. Mo doping enhances structural stability, enabling wide pH applicability. Electron transfer from Ni 3 S 2 nanoparticles to Ni single atoms accelerates kinetics and boosts intrinsic activity, which improves HER performance. Theoretical calculations confirm that Ni single atoms possess ideal H∗ adsorption energy, which optimizes H∗ adsorption capability of Ni 3 S 2 . This work offers suggestions for creating excellent low-cost electrolytic water catalysts.
研究领域:
电化学
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催化
·
材料科学
·
纳米技术
·
能量转换
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Hong-Rui Zhu,Xi-Lun Wang,Juan-Juan Zhao,Meng-Han Yin,Hui-Min Xu,Gao-Ren Li
Plastics are ubiquitous in human life and pose certain hazards to the environment and human body. The increasing amount of CO 2 in the atmosphere will lead to the greenhouse effect. Therefore, it is urgent to treat microplastic waste and CO 2 by using environmentally friendly and efficient technologies. In this work, we developed an efficient photoelectrocatalytic system composed of Ni single atoms (Ni SAs) supported by P, N-doped amorphous NiFe 2 O 4 (Ni SAs/A-P-N-NFO) as anode and Ag nanoparticles (Ag NPs) supported by CuO/Cu 2 O nanocubes (Ag NPs@CuO/Cu 2 O NCs) as cathode for microplastic oxidation and CO 2 reduction. The Ni SAs/A-P-N-NFO was synthesized by calcination-H 2 reduction method, and it achieved a Faraday efficiency of 93% for the oxidation reaction of poly (ethylene terephthalate) (PET) solution under AM 1.5 G light. As a photocathode, the synthesized Ag NPs@CuO/Cu 2 O NCs was utilized to reduce CO 2 to ethylene and CO at 1.5 V vs . RHE with selectivity of 42% and 55%, respectively. This work shows that the photoelectrocatalysis, as an environmentally friendly technology, is a feasible strategy for reducing the environmental and biological hazards of light plastics, as well as for efficient CO 2 reduction.
研究领域:
环境科学
·
材料科学
·
电化学
·
纳米技术
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2023
·
IF 10.9
Hao Wang,Jiangwen Liao,Jiajun Zhong,Yunpeng Liu,Lei Yao,Lixiong Qian,Yuecheng Lai,Xin Wang,Yikun Li,Jianxin Song,Xueqing Xing,Guang Mo,Zhongjun Chen,Zhonghua Wu
In this paper, the unclear Ni atom coordination structure evolution in one-pot pyrolysis method synthesizing Ni single atom catalyst using graphitic carbon nitride as support (Ni-g-C 3 N 4 ) was deeply discussed. In-situ X-ray absorption fine structure spectra and other assisted methods were used to characterize the structural evolution. The results demonstrate that the pyrolysis process can be divided into three stages. In the first stage from room temperature to 183 °C (Stage I), the NiCl 2 ⋅6H 2 O was mixed with the supporting material (dicyandiamide) to form the precursor with Ni-(H 2 O) 6 octahedral coordination configuration. In the second stage from 183 to 350 °C (Stage II), the H 2 O molecules have been removed and the supporting material was converted to melamine. The melamine molecules were polycondensed to melem during 308–350 °C. The intermediates labeled Ni-melamine and Ni-melem was formed with Ni-N 4 planar quadrilateral coordination configuration. In the third stage from 350 to 600 °C (Stage III ), the supporting material (melem) was gradually converted to g-C 3 N 4 , and the Ni-N 4 coordination configurations were replaced by Ni-N 6 planar hexagon coordination configuration one by one. The three Ni coordination configurations were further confirmed by Reverse Monte Carlo simulations and ab initio calculations .
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ye Wang,Yingkui Yan,Huabin Zhang,Xinsheng Peng,Hubiao Huang,Songtao Zhang,Li Shi
The development of unique single-atom catalysts with electron-rich feature is essential to promoting the photocatalytic CO 2 reduction, yet remains a big challenge. Here, a conceptionally new single-atom catalyst constructed from atomically dispersed Ni–P 3 species on black phosphorus (BP) nanosheets (BP-Ni) is synthesized for realizing highly efficient visible-light-driven CO 2 reduction when trapping photogenerated electrons from homogeneous light absorbers in the presence of triethanolamine as the sacrificial agent. Both the experimental and theoretical calculation data reveal that the Ni–P 3 species on BP nanosheets own the electron-rich feature that can improve the photogenerated charge separation efficiency and lower the activation barrier of CO 2 conversion. This unique feature makes BP-Ni exhibit the much higher activity as cocatalyst in the photocatalytic CO 2 reduction than BP nanosheets. The BP-Ni can also be applied as a cocatalyst for enhanced photocatalytic CO 2 reduction after combining with CdSe/S colloidal crystal photocatalyst. The present study offers valuable inspirations for the design and construction of effective catalytic sites toward photocatalytic CO 2 reduction reactions.
研究领域:
材料科学
·
催化
·
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Zhiwen Xu,Guangyu Chen,Fei Yang,Juhee Jang,Guimei Liu,Fei Xiao,Yan Sun,Xiaoyi Qiu,Weiwei Chen,Dong Su,Meng Gu,Minhua Shao
The development of inexpensive and high-performance bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of crucial significance for rechargeable metal-air batteries , but remains challenging. Herein, we report an ingenious bifunctional oxygen electrocatalyst integrating ZIF-derived carbon-anchored Fe/Ni single atoms, FeNi alloy nanoparticles , and graphene support (denoted as Fe/Ni-NC||FeNi@G). Synergizing highly active Fe single atoms for the ORR and highly efficient FeNi alloy nanoparticles for the OER, the as-constructed Fe/Ni-NC||FeNi@G catalyst exhibits outstanding bifunctionality; the potential gap between the OER potential at 10 mA cm –2 and the ORR half-wave potential is only 0.618 V, outperforming the benchmark Pt/C + Ir/C catalyst and most transition metal-based bifunctional catalysts reported in the literature. More importantly, the Fe/Ni-NC||FeNi@G-driven zinc-air battery (ZAB) delivers a maximum power density of ∼200 mW cm –2 , a specific capacity of 876 mAh g –1 , and excellent cycling stability with negligible voltage decay up to 500 hours (3000 cycles). This work provides an effective approach to designing highly efficient non-noble metal multifunctional catalysts for practical applications in rechargeable metal-air batteries.
研究领域:
材料科学
·
电化学
·
能源存储
·
催化
✓ 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）