ACS Catalysis
·
2023
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IF 12.9
Xu Yu,Han Tian,Zhengqian Fu,Fenglai Pei,Lingxin Peng,Ge Meng,Fantao Kong,Yafeng Chen,Chang Chen,Ziwei Chang,Xiangzhi Cui,Jianlin Shi
The hydrogen spillover effect on metal-supported electrocatalysts is of great significance in hydrogen-involved reactions, especially in a hydrogen oxidation reaction (HOR). Herein, a facile thermal reduction method has been adopted to synthesize W18O49 (WO2.72) nanospheres decorated with single nickel atoms, and the obtained Ni-WO2.72-T (1.20 wt % Ni) was used as a probe catalyst for investigating the hydrogen spillover effect, which exhibits enhanced HOR performance, stability, and resistance to CO poisoning in acidic electrolytes. Based on in situ Raman spectroscopy and the density functional theory (DFT) calculation, a synergistic effect between Ni single-atom active sites and the hydrogen spillover effect is proposed to contribute to the HOR performance on Ni-WO2.72-T. Briefly, the introduction of single Ni atoms induces electron redistribution on Ni-WO2.72-T, making Ni atoms positively charged for H2 adsorption and activation, and on the other hand, the reversible phase transformation between WO2.72 and HxWO2.72 facilitates H* transfer from Ni to WO2.72, i.e., hydrogen spillover, resulting in elevating the HOR catalytic activity. Both experimentation and theoretical calculations demonstrate that the reversible phase transformation of the WO2.72 substrate strengthens the hydrogen spillover effect and thus elevates the HOR catalytic performance, which is believed to be helpful in designing highly active catalysts for hydrogen-involving reactions.
研究领域:
电化学
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催化材料
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理论计算
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 11
·6122-6128
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IF 12.732
Wenxiu Ma,Zhe Chen,Jun Bu,Zhenpeng Liu,Jinjin Li,Chen Yan,Lin Cheng,Lei Zhang,Hepeng Zhang,Jichao Zhang,Tao Wang,Jian Zhang
In pursuit of environmental friendliness and high economic efficiency, renewable energy-driven selective acetylene semihydrogenation under ambient conditions is urgently required but remains a grand challenge. Herein, we explore single-atom nickel (Ni) dispersed N-doped carbon (SA-Ni-NC) as a novel electrocatalyst for catalyzing selective acetylene semihydrogenation. In situ electrochemical Raman and theoretical investigations reveal that weak π-adsorption of ethylene on individual Ni sites in SA-Ni-NC facilitates its desorption and thus avoids its overhydrogenation. Eventually, under pure acetylene flow, SA-Ni-NC exhibits a high ethylene faradaic efficiency (FEethylene) of 91.3% and a large current density of −92.2 mA cm−2 at −0.6 V vs. the reversible hydrogen electrode (RHE). Even in crude ethylene stream containing 1% acetylene impurities (1 × 104 ppm), SA-Ni-NC still manifests a high acetylene conversion of 97.4% with a large space velocity (SV) of 2.4 × 104 mL gcat−1 h−1 and a high turnover frequency (TOF) of 22.9 h−1 for each Ni atom.
研究领域:
材料科学
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电化学
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催化反应
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Hongyuan Chuai,Haibei Yang,Sheng Zhang
Ni single-atom-decorated nitrogen-doped carbon materials (Ni–Nx-C) have demonstrated high efficiency in the electrochemical reduction of CO2 (CO2RR) to CO. In this study, Ni–Nx-C active sites were embedded within a carbon membrane via an electrospinning and pyrolysis process. The resulting self-supported carbon membrane hosting Ni–Nx-C sites could be directly utilized as an electrode for the CO2RR. To enhance the CO2RR performance of the carbon membrane, the porous structure of the carbon membrane was fine-tuned by incorporating a pore-forming agent. The optimized porous carbon membrane electrode, K0.66-Ni-NC, achieved an impressive CO faradaic efficiency (FECO) of over 90% within a wide potential range from −0.8 to −1.6 V vs RHE for CO2RR. Additionally, it maintained an FECO of above 90% at −0.8 V vs RHE throughout a 30 h durability test in an H-cell. Further analysis has revealed that the porous structure of the carbon membrane not only facilitates the mass transport of CO2 but also increases the level of exposure of active sites during the CO2RR.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
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2020
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IF 7.216
Jingwen Pan,Gongxin Zhang,Zhongjie Guan,Qianyu Zhao,Guoqiang Li,Jianjun Yang,Qiuye Li,Zhigang Zou
Structure manipulation of photocatalysts at an atomic scale is a promising way to improve its photocatalytic performance. Herein, we realize the anchoring of single Ni atoms on the ZnIn 2 S 4 nanosheets with rich sulfur vacancies. Experimental results demonstrate that single Ni atoms induce the formation of Ni-O-M (Zn/In) atomic interface, which can efficiently promote the carriers separation and prolong the carrier life time. In addition, in situ electron spin resonance spectroscopy (ESR) confirms that the single Ni atoms act as an electron trapping center for protons reduction. As a result, the single Ni atoms decorated ZnIn 2 S 4 nanosheets with rich sulfur vacancies (Ni/ZnIn 2 S 4 -RV s ) shows a hydrogen evolution rate up to 89.4 μmol h −1 , almost 5.7 and 2.3 times higher compared to that of ZnIn 2 S 4 nanosheets with poor sulfur vacancies and rich sulfur vacancies (denoted as ZnIn 2 S 4 -PV s and ZnIn 2 S 4 -RV s ). This work opens up a new perspective manipulating the single-atom cocatalyst and sulfur vacancy on sulfide supports for improving photocatalytic hydrogen evolution.
研究领域:
材料科学
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光催化
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能源化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Xue Zhao,Zhu Zhu,Yingnan He,Haibo Zhang,Xiaohai Zhou,Wanbiao Hu,Meng Li,Shusheng Zhang,Yemin Dong,Xun Hu,Artem V. Kuklin,Glib V. Baryshnikov,Hans Ågren,Thomas Wågberg,Guangzhi Hu
Electrochemical synthesis of ammonia driven by clean energy is expected to realize the supply of ammonia for distributed production of industry and agriculture. Here, nickel nanoparticles and nickel in the form of single atoms were simultaneously anchored on the electrochemically active carrier BCN matrix through a structured domain strategy, which realized a high-efficiency, high-value-added, conversion of nitrate in sewage. Specifically, the electrochemical nitrate reduction reaction (NIRR) driven by BCN@Ni in alkaline media achieves an ammonia yield rate as high as 2320.2 μg h −1 cm −2 (at −0.5 V vs RHE), and Faraday efficiency as high as 91.15% (at −0.3 V vs RHE). Even in neutral and acidic media, the ammonia yield rates of NIRR driven by BCN@Ni are as high as 1904.2 μg h −1 cm −2 and 2057.4 μg h −1 cm −2 , respectively (at −0.4 V vs RHE). The 15 NO 3 - isotope labeling experiment verified that the recorded ammonia all came from the electrochemical reduction of NO 3 – on BCN@Ni. Density functional theory (DFT) calculations show that both nano-Ni and single-atom Ni in BCN@Ni have the ability to electrochemically convert NO 3 – into NH 3 , and that the addition of BCN can further promote the NIRR on Ni.
研究领域:
环境科学
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材料科学
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电化学
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产品关联
DOI
高影响因子
ChemSusChem
·
2023
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IF 8.4
Pu Zhang,Haihua Zeng,Decai Wen,Xiaoyu Sui,Zhuan Wang,Ying Wang,Hailong Chen,Yuxiang Weng,Jinlin Long
Graphical With the combination of surface organometallic chemistry and post-synthetic ligand exchange or calcination, the coordination environments of Ni sites were precisely manipulated to achieve a splendid improvement in hydrogen evolution reaction (HER) under visible-light irradiation. Thereinto, the 2,2′-bipyridine bonded Ni catalyst showed the optimum HER ability, 260 folds as Ni without ligand and 2.5 folds as 2-phenylpyridine bonded Ni catalyst. Solar hydrogen production at a high efficiency holds the significant importance in the age of energy crisis, while the micro-environment manipulation of active sites on photocatalysts plays a profound role in enhancing the catalytic performance. In this work, a series of well-defined single-site Ni-grafted TiO 2 photocatalysts with unique and specific coordination environments, 2,2′-bipyridine-Ni−O−TiO 2 (T−Ni Bpy) and 2-Phenylpyridine-Ni−O−TiO 2 (T−Ni Phpy), were constructed with the methods of surface organometallic chemistry combined with surface ligand exchange for visible-light-induced photocatalytic hydrogen evolution reaction (HER). A prominent rate of 33.82 μmol ⋅ g −1 ⋅ h −1 and a turnover frequency of 0.451 h −1 for Ni are achieved over the optimal catalyst T−Ni Bpy for HER, 260-fold higher than those of Ni−O−TiO 2 . Fewer electrons trapped oxygen vacancies and a larger portion of long-lived photogenerated electrons (>3 ns, ~52.9 %), which were demonstrated by the electron paramagnetic resonance and femtosecond transient IR absorption, correspond to the photocatalytic HER activity over the T−Ni Bpy. The number of long-lived free electrons injected from the Ni photoabsorber to the conduction band of TiO 2 is one of the determining factors for achieving the excellent HER activity.
研究领域:
材料科学
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催化化学
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能源科学
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2025
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IF 2.5
Yuting Li,Dandan Wang,Yuqin Ma,Fangbin Liu,Hongji Li,Qigming Xu,Haijiao Xie
The reduction of carbon dioxide (CO2) using electrochemical methods is one of the ways to achieve carbon recycling, as the increase in carbon dioxide emissions causes environmental problems. Single-atom dispersed Ni-NC site catalysts have emerged as effective electrocatalysts for the reduction of CO2 to CO. Using ZIF-8 as a carrier, we aim to design a high-performance single nickel-site catalyst by elucidating the structure evolution of NiNx sites during thermal activation as well as other key external factors such as the carbon particle size and nickel content. The pyridine N active sites generated after calcination have higher activity and CO selectivity. The catalyst achieved up to 99.6% CO generation at −0.88 V vs. RHE, and is one of the best catalysts for the reduction of CO2 to CO. This work demonstrates an effective method for designing efficient electrochemical CO2 reduction catalysts by tuning the surface structure of single-atom anchored carriers.
研究领域:
材料科学
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环境科学
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电化学
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Lingyue Liu,Peng Zhou,Xiaozhi Su,Yuhang Liu,Yuhan Sun,Hongbin Yang,Heyun Fu,Xiaolei Qu,Shantang Liu,Shourong Zheng
Monitoring sulfur dioxide (SO 2 ) in the environment requires a sensor to feature adequate sensitivity, selectivity, and low detection levels. Herein, we report an ultrasensitive, low-concentration SO 2 gas sensor that employs single atoms nickel anchored on oxygen vacancy-rich SnO 2 nanorods (SAC-Ni/H-SnO 2 ) as the sensing material. The response value of the SAC-Ni/H-SnO 2 sensor to 20 ppm SO 2 is 48, and the detection limit is 100 ppb, which is superior to most of reported SO 2 sensors. In-situ DRIFTS and ESR characterization shows that the coupling effects of SAC-Ni and adjacent oxygen vacancy on SnO 2 surface, which promote the adsorption of SO 2 and activation of chemisorbed oxygen, respectively. This effective single-atom catalyst provides a new insight into complex gas sensing mechanisms and demonstrates a promising approach of using single-atom catalysts for gas sensing applications.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2023
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IF 10.9
Songyu Yang,Kailin Wang,Qiao Chen,Yan Wu
S-scheme heterostructure photocatalysts can achieve highly efficient solar energy utilization. Here, single-atom Ni species were deposited onto TiO 2 /g-C 3 N 4 (TCN) composite photocatalyst with an S-scheme heterojunction for highly efficient photocatalytic water splitting to produce hydrogen. Under solar irradiation, it realized the hydrogen production activity of 134 µmol g –1 h –1 , about 5 times higher than the TCN without atomic Ni. In-situ Kelvin probe force microscopy characterization and the density functional calculation certify that by forming the S-scheme heterojunction, the photo-excited electrons from the TiO 2 combine with the photogenerated holes at the coupled g-C 3 N 4 driven by a built-in electric field. More importantly, the single-atom Ni species stabilized the photogenerated electrons from the g-C 3 N 4 could effectively enhance the charge separation between the holes on the valence band of TiO 2 and electrons at the conduction band of g-C 3 N 4 . Meanwhile, the Ni atoms act as the surface catalytic centers for the water reduction reaction, which greatly improves the reactivity of the photocatalyst. The present work provides a new approach for developing noble metal-free heterojunctions for high-efficiency photocatalysis.
研究领域:
材料科学
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能源化学
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催化科学
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2024
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IF 14.4
Jiyue Zhang,Wenda Wang,Xiaowei Chen,Jinlong Jin,Xiaojun Yan,Jianmei Huang
As an efficient and clean energy carrier, hydrogen is expected to play a key role in future energy systems. However, hydrogen-storage technology must be safe with a high hydrogen-storage density, which is difficult to achieve. MgH2 is a promising solid-state hydrogen-storage material owing to its large hydrogen-storage capacity (7.6 wt %) and excellent reversibility, but its large-scale utilization is restricted by slow hydrogen-desorption kinetics. Although catalysts can improve the hydrogen-storage kinetics of MgH2, they reduce the hydrogen-storage capacity. Single-atom catalysts maximize the atom utilization ratio and the number of interfacial sites to boost the catalytic activity, while easy aggregation at high temperatures limits further application. Herein, we designed a single-atom Ni-loaded TiO2 catalyst with superior thermal stability and catalytic activity. The optimized 15wt%-Ni0.034@TiO2 catalyst reduced the onset dehydrogenation temperature of MgH2 to 200 °C. At 300 °C, the H2 released and absorbed 4.6 wt % within 5 min and 6.53 wt % within 10 s, respectively. The apparent activation energies of MgH2 dehydrogenation and hydrogenation were reduced to 64.35 and 35.17 kJ/mol of H2, respectively. Even after 100 cycles of hydrogenation and dehydrogenation, there was still a capacity retention rate of 97.26%. The superior catalytic effect is attributed to the highly synergistic catalytic activity of single-atom Ni, numerous oxygen vacancies, and multivalent Tix+ in the TiO2 support, in which the single-atom Ni plays the dominant role, accelerating electron transfer between Mg2+ and H– and weakening the Mg–H bonds. This work paves the way for superior hydrogen-storage materials for practical unitization and also extends the application of single-atom catalysis in high-temperature solid-state reactions.
研究领域:
储能技术
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催化化学
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材料科学
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纳米技术
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氢能技术
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固态化学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
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IF 14.7
Ren Yuqi,Fu Yiwei,Li Naixu,You Changjun,Huang Jie,Huang Kai,Sun Zhenkun,Zhou Jiancheng,Si Yitao,Zhu Yuanhao,Chen Wenshuai,Duan Lunbo,Liu Maochang
H 2 O dissociation plays a crucial role in solar-driven catalytic CO 2 methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO 2 catalyst with single-atom Ni anchored around its surface V o sites by replacing Ce atoms to promote H 2 O dissociation and achieve effective photothermal CO 2 reduction under concentrated light irradiation. The high photon flux reduces the apparent activation energy for CH 4 production and prevents V o from depletion. The defects coordinated with single-atom Ni, significantly promote the capture of charges and local phonons at the Ni d -impurity orbitals, thereby inducing more effective H 2 O activation. The catalyst presents a CH 4 yield of 192.75 µmol/cm 2 /h, with a solar-to-chemical efficiency of 1.14% and a selectivity ~100%. The mechanistic insights uncovered in this study should help further the development of H 2 O-activating catalysts for CO 2 reduction and thereby expedite the practical utilization of solar-to-chemical technologies.
研究领域:
催化
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太阳能
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Sun Yining,Fan Kui,Li Jinze,Wang Lei,Yang Yusen,Li Zhenhua,Shao Mingfei,Duan Xue
The electrochemical oxygen reduction reaction (ORR) to produce hydrogen peroxide (H 2 O 2 ) is appealing due to its sustainability. However, its efficiency is compromised by the competing 4e − ORR pathway. In this work, we report a hierarchical carbon nanosheet array electrode with a single-atom Ni catalyst synthesized using organic molecule-intercalated layered double hydroxides as precursors. The electrode exhibits excellent 2e − ORR performance under alkaline conditions and achieves H 2 O 2 yield rates of 0.73 mol g cat −1 h −1 in the H-cell and 5.48 mol g cat −1 h −1 in the flow cell, outperforming most reported catalysts. The experimental results show that the Ni atoms selectively adsorb O 2 , while carbon nanosheets generate reactive hydrogen species, synergistically enhancing H 2 O 2 production. Furthermore, a coupling reaction system integrating the 2e − ORR with ethylene glycol oxidation significantly enhances H 2 O 2 yield rate to 7.30 mol g cat −1 h −1 while producing valuable glycolic acid. Moreover, we convert alkaline electrolyte containing H 2 O 2 directly into the downstream product sodium perborate to reduce the separation cost further. Techno-economic analysis validates the economic viability of this system.
研究领域:
电化学
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催化
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材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）