ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Ziqiang Wang,Zechuan Dai,Hongjie Yu,Hugang Zhang,Wenjing Tian,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Electrochemical ammonia synthesis is considered as an alternative sustainable method to the traditional Haber–Bosch process because of the reduced energy consumption and mild operation conditions. The key is to design efficient electrocatalysts for facile adsorption and activation of nitrogen. Herein, a nanoporous Pd film with a tunable pore size has been in situ grown on Ni foam (nPd/NF) via a micelle-assisted replacement method using NF as a reductant and substrate, where polystyrene-b-poly(ethylene oxide) and 1,3,5-triisopropylbenzene serve as a pore-forming agent and a swelling agent, respectively. Combining the continuous large nanoporous structure and self-supported properties, the obtained nPd/NF exhibits excellent catalytic performance for ammonia synthesis with a high NH3 yield of 18.27 μg h–1 mgcat–1 and a faradaic efficiency of 10.36% in 0.1 M Na2SO4. This work provides a fascinating route for the rational design of self-supported porous noble metals with a tunable pore size for effective electrosynthesis of ammonia.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
DOI
高影响因子
Materials Today Physics
·
2022
·
IF 11.021
Mengjie Sun,Chaoqun Ma,Min Ma,Yanjiao Wei,Shihua Dong,Xiaoli Zhang,Jian Tian,Minhua Shao
Electrocatalytic nitrogen reduction (NRR) is regarded as an energy-efficient technology to produce NH 3 . Nevertheless, achieving high NH 3 yield and Faradaic efficiency (FE) under ambient conditions remains a great challenge. Herein, 1T/2H mixed-phase MoS 0·5 Se 1.5 (named 1T/2H MoSSe) nanoflower, as an efficient non-noble metal NRR electrocatalyst, was synthesized by the one-step solvothermal method. 1T/2H MoSSe realizes an excellent NH 3 yield of 32.32 μg h −1 mg cat. −1 at −0.45 V vs. RHE and an outstanding FE of 12.66% at −0.40 V vs. RHE in 0.1 M HCl, which are better than pure MoS 2 (NH 3 yield: 15.16 μg h −1 mg cat. −1 , FE: 0.35%) and MoSe 2 (NH 3 yield: 26.42 μg h −1 mg cat. −1 , FE: 2.75%). Density functional theory (DFT) calculations exhibit that MoSSe catalyst is structurally favorable to the potential-determining step (PDS, *NH–NH 2 → *NH 2 –NH 2 ) and thus shows increased NRR activity and selectivity. A promising tactic for the rational design of economical, efficient, and durable NRR electrocatalysts is proposed in this work.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xinshan Rong,Haifei Chen,Jian Rong,Xiaoying Zhang,Jing Wei,Shuang Liu,Xiangtong Zhou,Jicheng Xu,Fengxian Qiu,Zhiren Wu
In this report, environmental and energy issues were deal with a Z-scheme photocatalytic system toward the synthetic ammonia by N 2 photofixation. Different from traditional double-charge-transfer model, a direct all-solid-state Z-scheme system of modified TiO 2 (MT) loaded with ZnFe 2 O 4 (ZFO) was obtained by solvothermal-calcination method, in which calcination temperature is crucial for the mesoporous structure and formation of Z-scheme TiO 2 /ZnFe 2 O 4 . At ambient temperature and pressure, the MT/ZFO photocatalyst presented the ammonia generation rate of about 1.48 μmol/L/min, which is higher than that of single MT or ZFO. The photocatalytic activity enhancement of ammonia generation was attributed to the Z-scheme charge transfer model with a more negative reduction potential in the conduction band of ZnFe 2 O 4 . Combining the commonly TiO 2 and ZnFe 2 O 4 by a special method shows a desirable Z-scheme photocatalytic system, which can be extended to the fabrication of other Z-scheme photocatalyst according to the various application need.
研究领域:
环境科学
·
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Hongjing Wang,Dandan Yang,Songliang Liu,Shuli Yin,You Xu,Xiaonian Li,Ziqiang Wang,Liang Wang
The Au catalyst is attractive for electrochemical ammonia synthesis. The design of Au catalyst with favorable morphology and composition is significant for enhancing its performance. Herein, an effective and universal synthetic method is proposed to fabricate unique metal–nonmetal AuPdP nanowires (AuPdP NWs), which is simply performed by the solvothermal reaction of Au nanowires with Pd(PPh3)4. The facile hydrogen adsorption at Pd sites and weak binding to Au sites favor the selective hydrogenation of N2 to NH3. Moreover, phosphorus doping provides more sites for the nitrogen reduction reaction due to its rich valence electrons. Therefore, the AuPdP NWs exhibit superior electrocatalytic performance for electrochemical ammonia synthesis with high NH3 yield, faradic efficiency, and stability. The presented synthetic method provides an attractive strategy for the simultaneous incorporation of Pd and P into metallic catalysts with controlled morphology for various electrocatalytic applications.
研究领域:
材料科学
·
电催化
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2019
·
IF 6.395
Lingling Qiao,Guoyi Duan,Sheng Zhang,Yuan Ren,Yanzhi Sun,Yang Tang,Pingyu Wan,Ran Pang,Yongmei Chen,Armistead G. Russell,Maohong Fan
Electrochemical ammonia synthesis is regarded as a green, clean, and sustainable technology alternative to the Haber-Bosch process to reduce fossil fuel consumption and greenhouse gas emission . In this research, an earth-abundant CoFe layered double hydroxide was prepared with a simple one-step hydrothermal method and was employed as a promising catalyst for electrochemical ammonia synthesis. The CoFe double hydroxide exhibited excellent catalytic activity with a high generation rate of 1.1 × 10 −9 mol s −1 cm −2 in a single-chamber cell, and a high Faradaic efficiency of 14.18% was obtained when the concentration of protons and electrons was limited in a double-chamber cell. The outstanding catalytic performance of CoFe layered double hydroxide was attributed to the abundant N 2 adsorption sites provided by the binder-free three-dimensional nano-structure and the synergy between the Co and Fe atoms in the layer. A microkinetic model of electrochemical ammonia synthesis catalyzed with CoFe layered double hydroxide was proposed, which was consistent with the experimental results. A possible ammonia synthesis mechanism was proposed based on the experiments and theoretical calculations.
研究领域:
材料科学
·
环境科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Ruonan Li,Runlin Ma,Li-Li Zhang,Wei Ma,Gonglei Shao,Xu Zhang,Yun Tian,Menggai Jiao,Zhen Zhou
To tackle the challenge in electrochemical nitrogen fixing and reduction in aqueous electrolytes, the conventional approach has been to suppress the competitive hydrogen evolution reaction. Nonetheless, proton provision is a crucial step in the nitrogen reduction pathway to produce ammonia, and a single active site faces the daunting task in striking a balance between high nitrogen fixation efficiency and fast protonation kinetics. This work presents a harmonic strategy featuring atomically dispersed dual Fe–Mo sites anchored in an N-doped carbon (FeMoNC) substrate, where a low-spin Fe center with enriched empty d orbitals aids in nitrogen fixation and activation, and the adjacent Mo site accelerates the protonation kinetics of N-containing intermediates at the Fe site via a distal associative mechanism. Driven by this co-catalytic mechanism, the FeMoNC catalyst achieves a Faradaic efficiency of 37.42%, marking a significant improvement of 7.8- and 10.6-fold over Fe or Mo single-atom catalysts, respectively. Furthermore, an excellent NH3 yield of 54.40 μg h–1 mgcat.–1 is realized in a flow cell by enhancing mass transfer. This study provides valuable insights into diatomic co-catalytic mechanisms for electrochemical ammonia synthesis.
研究领域:
材料科学
·
催化化学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Xue Zhao,Xiuxiu Jia,Haibo Zhang,Xiaohai Zhou,Xiao Chen,Huaisheng Wang,Xun Hu,Jian Xu,Yingtang Zhou,Hucai Zhang,Guangzhi Hu
Electrochemical nitrate reduction reaction (NIRR) driven by sustainable energy is not only expected to realize the green production of ammonia under ambient conditions, but also a promising way to purify nitrate wastewater. The ammonia yield rate and Faradaic efficiency of NIRR catalyzed by Pd10Cu/BCN constructed with structural constraints and pre-embedded reducing agent strategies were as high as 102,153 μg h −1 mg cat. −1 and 91.47%, respectively. Pd10Cu/BCN can remove nearly 100% of 50 mg L −1 NO 3 - without NO 2 - residue within 10 h, and the realization of this effect does not require the participation of any chloride. Control experiments and DFT calculations explain the efficient operation mechanism of NIRR on Pd10Cu/BCN, where the Pd and CuN4 sites play the role of synergistic catalysis. Compared with the reported literature, Pd10Cu/BCN with good biocompatibility has become an outstanding representative of NIRR catalyst, which provides an alternative way for the green production of ammonia and the purification of nitrate wastewater.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Jieying Wan,Ji Yang,Na Yang,Yifei Sun,Chuansheng Hu,Yang Zhao,Xiaoyan Xu,Haifeng Qi,Xiaodong Li,Hao Zhang
Electrochemical nitrate reduction reaction (NO3–RR) presents a sustainable method for ammonia synthesis. Single-atom catalysts possessing the symmetric planar four-ligand structure (M-N4) serve as advantageous catalytic active sites for NO3–RR. However, the inherent extreme symmetry of the standard M-N4 structure limits the reaction kinetics. Herein, we introduce a symmetry-breaking iron single-atom catalyst coordinated with axial chlorine on nitrogen-doped carbon (Cl-Fe-NC) for NO3–RR. Cl-Fe-NC exhibits a 99.4% ammonia Faradaic efficiency (FE) at −0.28 V vs reversible hydrogen electrode (RHE) with a 9396.7 μgNH3 h–1 cm–2 yield rate at −0.68 V vs RHE, remarkably surpassing that of Fe-NC (<80%, 4330.9 μgNH3 h–1 cm–2 at the same potential). Operando synchrotron radiation Fourier transform infrared (SR-FTIR) spectroscopy confirms that key intermediates, such as *NO, *NO-Hx, and σ(N–H), are formed. Density functional theory (DFT) calculations attribute the optimized free energy of NO3–RR intermediates to the axial chlorine design, reducing the potential determination step barrier energy by up to 0.66 eV. The presence of axial Cl atoms modulates the symmetry of the single Fe atom, enhancing the adsorption of nitrate ions and the enrichment of critical intermediates during NO3–RR while inhibiting the hydrogen evolution reaction (HER). This discovery opens avenues for boosting electrochemical ammonia synthesis through the precise modulation of atomic structures by doping heteroatoms for symmetry breaking.
研究领域:
催化化学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Wenwen Cai,Yuyao Sun,Yanyun Zhang,Hongdong Li,Yaodong Yu,Jianping Lai,Lei Wang
In the field of electrocatalytic nitrogen reduction reaction (NRR), molten salt is used as a unique electrolyte due to its advantages of high N 2 solubility and wide electrochemical window. However, it has failed to be widely used due to its high reaction temperature (mostly > 200 °C) and low yield. Herein, a novel low-temperature (<100 °C) electrolysis system with hydrated molten salt hybrid electrolyte is designed. This system exhibits an ammonia yield of 1.003 × 10 −8 mol s −1 cm −2 (−0.7 V vs. SCE) at 60 °C. Faradaic efficiency (FE) reaches 80.45 % (−0.65 V vs. SCE). The NH 3 yield and FE are increased by 18.6 and 2 times compared to the previously reported low-temperature system, respectively. Linear sweep voltammetry (LSV), in situ Raman and in situ Fourier Transform-Infrared (FT-IR) experiments show that solid crystalline water can be used as a hydrogen source to effectively promote NRR while inhibiting the hydrogen evolution reaction (HER). Molecular dynamics (MD) experiments confirm that the electrolyte system maintains a high N 2 solubility and mass transfer rate.
研究领域:
化学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Guan Sheng,Yudong Jiang,Zirong Yan,Jinshu Tian,Shaobo Tu
MXenes represent exceptionally promising electrocatalytic materials for ammonia synthesis, owing to their outstanding electrical conductivity, modifiable surface functional groups, exceptional hydrophilicity, high specific surface area, and electronegative surface characteristics. In this investigation, we systematically demonstrate that the persistent challenge of Cu and Co nanoparticle agglomeration can be effectively addressed through the in-situ growth of bimetallic CuCo nanoparticles on Ti 3 C 2 T x MXene nanosheets. This innovative approach significantly enlarges the electrochemically active surface area, maximizes the exposure of catalytically active sites, and optimizes mass transport properties, consequently leading to substantially enhanced electrocatalytic performance for ammonia synthesis. Among the series of Cu x Co y /MXene composites developed, the Cu 2 Co 1 /MXene hybrid catalyst demonstrates superior nitrate reduction reaction (NO 3 RR) activity, achieving remarkable performance metrics including: An exceptional ammonia yield rate of 2.73 mg cm −2 h −1 at an applied potential of −0.85 V versus RHE, a high Faradaic efficiency of 72.05 %, and outstanding selectivity reaching 90.6 %. These breakthrough results establish new benchmarks for MXene-based electrocatalysts in sustainable ammonia production.
研究领域:
材料科学
·
电化学
·
催化
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2023
·Vol. 16
·期 8
·10770-10778
·
IF 9.9
Guan Renquan,Cheng Xueying,Chen Yunning,Wu Zhengkai,Zhao Zhao,Shang Qingkun,Sun Yingnan,Sun Zaicheng
Ammonia is an important chemical raw material and non-carbon-based fuel. Photocatalytic ammonia production technology as a mild alternative to the traditional Harbor–Bosch route is carried out at the air, liquid, and solid three-phase interface. Promoting the activation of N 2 , depressing hydrogen evolution reaction (HER), and increasing the local N 2 concentration around the catalyst surface are critical factors in achieving high conversion efficiency. In this paper, we proposed that defective TiO 2 is surface-modified by alkyl acids with different carbon chain lengths (C 2 , C 5 , C 8 , C 11 , and C 14 ) to tune the catalyst surface properties. The defect sites greatly promote N 2 adsorption and activation. The wettability of the catalyst can be regulated from hydrophilic to hydrophobic by the length of the alkyl chain. The hydrophobic surface enhances the N 2 adsorption and increases the local N 2 concentration due to its aerophile. Meanwhile, it depresses the proton adsorption and HER. Overall, the nitrogen reduction reaction (NRR) is greatly promoted. Among the series of samples, they present a systematic change and have a maximal NRR performance for n-octanoic acid-defective TiO 2 (C 8 -Vo-TiO 2 ; Vo = oxygen vacancy). The rate of ammonia production can be as high as 392 µmol·g −1 h −1 . This work provides a new strategy for efficient ammonia synthesis at the three-phase interface using photocatalyst technology.
研究领域:
光催化
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材料科学
·
化学工程
·
环境科学
·
表面化学
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Anquan Zhu,Heng Liu,Lulu Qiao,Bin Liu,Kunlun Liu,Chuhao Luan,Kai Liu,Yin Zhou,Dewu Lin,Guoqiang Gan,Jiapei Li,Guo Hong,Wenjun Zhang
The electrochemical nitrate reduction reaction (eNO 3 RR) is widely recognized as a promising strategy for sustainable ammonia production and supporting the nitrogen cycle. However, its advancement is impeded by complex behavior of reaction intermediates and the inevitable reconstruction of precatalysts. To address these challenges, the generation and utilization of active hydrogen (*H) are strategically managed by tailoring the RuO 2 /Co 3 O 4 precatalyst and optimizing the electrolyte composition (OH − and NO 3 − concentration), thereby selectively enhancing ammonia formation. Consequently, the in situ reconstructed RuO 2 /Co(OH) 2 catalyst achieves an impressive ammonia yield of 35.9 ± 0.9 mg h −1 cm −2 and a Faradaic efficiency (FE) of 98.1 ± 2.6% at −0.3 V versus RHE. Furthermore, the catalyst shows significant potential for applications in nitrate-rich wastewater treatment and rechargeable Zn-NO 3 − batteries, maintaining stable operation for over 260 hours at 1 mA cm −2 with only a 6 mV increase in the potential window. Mechanistic studies reveal that electron-rich RuO 2 facilitates *H generation through water dissociation, which subsequently migrates to Co(OH) 2 to hydrogenate nitrogenous intermediates, selectively producing ammonia. This study highlights the importance of designing efficient catalytic systems that address both precatalyst reconstruction and the complexities of reactant and intermediate conversion in electrolytes, which are essential for managing the intricate electron and proton transfer processes involved in eNO 3 RR.
研究领域:
电催化
·
环境催化
·
能源化学
·
材料化学
·
可持续化学
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废水处理
·
电化学工程
✓ 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）