Sustainability
·
2025
·Vol. 17
·期 9
·3835
·
IF 3.3
Qiufang Yao,Yanping Xiao,Haoqing Wang,Haobin Zhong,Tongtong Wang
The electrocatalytic reduction of nitrate (ERN) to ammonia offers a promising route to address energy shortages and environmental pollution, but its practical application is hindered by low selectivity due to complex eight-electron transfer pathways and high energy consumption (EC)from the kinetically sluggish oxygen evolution reaction (OER). This study proposes a dual strategy: (1) designing a multi-functional self-supported ANP electrode via vapor deposition to enhance ERN activity and (2) replacing the OER with thermodynamically favorable anodic reactions (urea oxidation reaction (UOR), sodium metabisulfite oxidation reaction (S(IV)OR), sulfite and urea oxidation reaction (S(IV)/UOR)) to reduceEC. The ANP cathode achieved a nitrate removal rate (R%) of 97.7%, ammonia selectivity (SE%) of 91.8%, and Faradaic efficiency (FE) of 97.3% at −1.2 V, with an ammonia yield of 0.0616 mmol h−1mg−1and anECof 8.239 kWh/kg, while in situ-generated atomic hydrogen (*H) was identified as key to improving nitrate removal and selectivity. Replacing the OER with alternative anodic reactions significantly improved system efficiency: the UOR reducedECby 17.5%, S(IV)OR saved 27.6% energy with 7.1% higher ammonia yield, and a hybrid S(IV)/UOR system achieved a 32.1% lowerECand a 12.6% greater ammonia yield than the OER. These differences stemmed from variations in cell voltage and ammonia production rates. This work provides a viable approach for selective nitrate-to-ammonia conversion and guides the design of energy-efficient electrocatalytic systems for sustainable nitrogen recovery.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 4
·3026-3033
·
IF 8.897
Sun Hao,Yin Hua-Qing,Shi Wenxiong,Yang Lu-Lu,Guo Xiang-Wei,Lin Hong,Zhang Jiangwei,Lu Tong-Bu,Zhang Zhi-Ming
Electrochemical nitrogen reduction reaction (NRR) under ambient conditions is highly desirable to achieve sustainable ammonia (NH 3 ) production via an alternative carbon free strategy. Single-atom catalysts (SACs) with super high atomic utilization and catalytic efficiency exhibit great potential for NRR. Herein, a high-performance NRR SAC is facilely prepared via a simple deposition method to anchor Au single atoms onto porous β-FeOOH nanotubes. The resulting Au-SA/FeOOH can efficiently drive NRR under ambient conditions, and the NH 3 yield reaches as high as 2,860 µg·h −1 ·mg Au −1 at −0.4 V vs. reversible hydrogen electrode (RHE) with 14.2% faradaic efficiency, much superior to those of all the reported Au-based electrocatalysts. Systematic investigations demonstrate that the synergy of much enhanced N 2 adsorption, directional electron export, and mass transfer ability in Au-SA/FeOOH greatly contributes to the superior NRR activity. This work highlights a new insight into the design of high efficient NRR electrocatalysts by combination of porous metal oxide matrix and highly active single-atom sites.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
Nature Sustainability
·
2022
·Vol. 6
·期 2
·169-179
·
IF 27.157
Zhang Shengbo,Han Miaomiao,Shi Tongfei,Zhang Haimin,Lin Yue,Zheng Xusheng,Zheng Li Rong,Zhou Hongjian,Chen Chun,Zhang Yunxia,Wang Guozhong,Yin Huajie,Zhao Huijun
The dominant Haber–Bosch process to produce ammonia, arguably the most important chemical in support of global food supply, is both energy and carbon intensive, resulting in substantial environmental impacts. Electrocatalytic nitrogen reduction reaction (NRR) powered by renewable electricity provides a green synthetic route for ammonia, but still suffers from insufficient yield rate and Faradaic efficiency. Single-atom electrocatalysts (SACs) have the potential to transform this catalytic process; however, controllable synthesis of SACs with high loading of active sites remains a big challenge. Here we utilize bacterial cellulose with rich oxygen functional groups to anchor iron (Fe) and cobalt (Co), realizing high density, atomically dispersed, bimetallic Fe–Co active sites. For electrocatalytic NRR, our catalyst design delivers a remarkable ammonia yield rate of 579.2 ± 27.8 μg h −1 mg cat. −1 and an exceptional Faradaic efficiency of 79.0 ± 3.8%. The combined theoretical and experimental investigations reveal that the operando change in coordination configuration from [(O-C 2 ) 3 Fe–Co(O-C 2 ) 3 ] to [(O-C 2 ) 3 Fe–Co(O-C)C 2 ] is the enabling chemistry. Our findings suggest a general approach to engineer SACs that can drive critical reactions of relevance for sustainability.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yu Tang,Pan Ran,Linjun Zhong,Haohong Liao,Qing Tong,Weixin Zou,Lin Dong
Electrochemically converting nitrate in wastewater as underleveraged nitrogen source into ammonia is a sustainable strategy for simultaneously valorizing wastewater and alleviating environmental contamination. However, it remains challenging for conversion of environmentally relevant nitrate in complex environments. Herein, a versatile IrCo alloy on N-doping carbon is presented with 93.3 % Faradaic efficiency and 21 mg h −1 mg cat −1 ammonia yield. Furthermore, we first achieve nearly complete nitrate removal (>99 %) under different pH conditions, from typical industrial wastewater concentrations (40 mM) to a drinking water standard (NO 3 – -N < 5 μg ml −1 ). Afterwards, high-value struvite (NH 4 MgPO 4 ·6H 2 O) products were obtained from the produced ammonia on a gram scale. DFT calculation reveals that optimized Co structure modulates the adsorption of intermediate *NH and facilitates further hydrogenation steps (*NH → *NH 2 ), whereas, limited on isolate Co sites due to weak H 2 O affinity and over-strong *H adsorption. The work gives effective insights into progressive ammonia production and environmental wastewater utilization.
研究领域:
环境科学
·
化学工程
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·
IF 10.7
Chunzheng Wu,Jingyuan Lin,Zhuojiong Xie,Xuan Kai,Xiao Yu,Zhenyu Yan,Jinwei Fang,Shanliang Chen,Jianzhong Guo,Wei Wang,Fengping Peng
Temperature fluctuations caused by sunlight represent a form of low-quality thermal energy that is generally insufficient for driving chemical reactions. Here, we designed a ZnO–MXene (Ti3C2) heterostructure catalyst, which can harvest solar near-infrared (NIR) energy to drive the sluggish ammonia production reaction using water and N2 as the feedstock. Our research confirmed that ammonia was produced through a pyroelectric process, rather than a photocatalytic process. The ZnO–MXene heterostructure with ∼20 wt% of Ti3C2 exhibited a 6.5-fold improvement in activity compared to bare ZnO. The Ti3C2 not only harvests NIR energy to heat up the pyroelectric ZnO, but also traps the pyro electrons from ZnO and co-catalyzes the reduction of N2 to ammonia. This work offers a novel strategy for ammonia production utilizing the abundant solar NIR energy under ambient conditions.
研究领域:
材料科学
·
催化化学
·
能源利用
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huiqun Cao,Bin Liang,Shenghua Ye,Ziqiong Zhuang,Lirong Zheng,Wenda Chen,Weibin Chen,Jie Zhang,Qinghao Zhang,Jianhong Liu,Xueqing Yan,Qianling Zhang
Conversion of NO 3 − -to-NH 3 via the electrocatalytic nitrate reduction reaction (NO 3 - RR) is an emerging strategy for ammonia production and storage of “green hydrogen”, but is limited by the dissatisfactory activity and selectivity. In this study, we discovered that cobalt carbonate hydroxide (Co 2 (OH) 2 CO 3 ) underwent a potential-induced self-reconstruction to cobalt hydroxide (Co(OH) 2 ) during NO 3 - RR. The incorporation of Ru into Co 2 (OH) 2 CO 3 expedited the aforementioned self-reconstruction process and resulted in the formation of Ru single-atomic sites (Ru SASs) anchored on Co(OH) 2 nanosheets. This structure is reported as a highly efficient electrocatalyst for NO 3 − -to-NH 3 conversion and exhibits exceptional electrochemical performance in zinc-NO 3 − batteries. Theoretical analysis revealed that the conversion of NO 3 − -to-NH 3 occurred on Ru SASs through an N-end pathway with *NO as a characteristic intermediate. Furthermore, Ru SASs facilitated the thermodynamic-determining step of *NH 2 -to-*NH 3 , thus promoting the overall NO 3 − -to-NH 3 conversion process.
研究领域:
材料科学
·
电化学
·
催化化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Shiyu Li,Jin Yan,Meihuan Liu,Hui Su
The electrochemical conversion of nitrate, a widespread water pollutant, into valuable ammonia represents a green and decentralized approach to ammonia synthesis. However, the sluggish multielectron-proton coupling path and the low reactive species (nitrate and proton) concentration at the catalyst interface inhibit the efficiency of ammonia production from nitrate reduction reaction (NitRR). Herein, we introduce a novel iron-based tandem catalyst encapsulated by reduced graphene oxide (denoted as Fe-rGO), with a superior ammonia production rate of 47.815 mg h −1 mg −1 cat and a high Faraday efficiency (FE) of 96.51% at an applied potential of −0.5 V. It also delivers a robust stability with FE above 90% under a current density of 250 mA cm −2 for 50 h. In situ X-ray absorption spectroscopy reveals that the FeO x is dynamically translated to Fe 0 site concurrently with the enhancement of the NH 3 production rate, suggesting the Fe 0 site as hydrogenation active center. The asymmetric distribution of surface charges of rGO not only enriches nitrate ions at the catalytic interface and promotes the hydrogenation process in NitRR, but also protects the iron species and ensures their stability during electrolysis. The Zn-NO 3 − battery demonstrates an impressive FE of 88.6%, highlighting its exceptional potential for practical applications.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·12041-12052
·
IF 3.553
Yi Xuerui,He Xiaobo,Yin Fengxiang,Yang Tong,Chen Biaohua,Li Guoru
The global NH 3 production is dominated by Haber–Bosch process, requiring high temperature and pressure. Electrochemical N 2 reduction reaction (NRR) under ambient conditions is a greener path for artificial N 2 fixation to NH 3 but calling for efficient catalyst to increase activity and selectivity. Herein, we report the iron-based metal–organic frameworks (MOFs), i.e., MIL-88B–Fe and amine-functionalized MIL-88B–Fe (NH 2 –MIL-88B–Fe) as efficient catalysts for electrochemical NRR under ambient temperature and pressure in neutral electrolyte. NH 2 –MIL-88B–Fe shows higher NH 3 yield rate of 1.205 × 10 –10 mol s −1 cm −2 than MIL-88B–Fe (3.575 × 10 –11 mol s −1 cm −2 ). Furthermore, NH 2 –MIL-88B–Fe exhibits the highest Faradaic efficiency of 12.45% at 0.05 V versus RHE. The control experiments prove that NH 3 is produced through electrocatalytic NRR. This work may trigger the interest of using MOFs as highly efficient catalysts for electrochemical NH 3 production.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Z. Wang,W. Tian,Z. Dai,P. Wang,Y. Xu,X. Li,L. Wang,H. Wang
Electrochemical synthesis of ammonia has attracted widespread attention because of its mild reaction conditions, low energy consumption, and no greenhouse gas generation, but suffers from low ammonia production rate and Faraday efficiency. Here, sulfur-modified silver telluride nanorods (S–Ag 2 Te NRs) have been synthesized as high-efficiency catalysts for the electrochemical synthesis of ammonia. The sulfur modification would offer higher adsorption energy for nitrogen intermediates and more active sites for the hydrogenation of nitrogen to ammonia. Therefore, the S–Ag 2 Te NRs show excellent electrocatalytic performance with an NH 3 yield of 26.44 μg h −1 mg −1 cat. and Faradaic efficiency of 17.48%, which is much higher than that of Ag 2 Te NRs. This work has opened an exciting sulfur-modified strategy to design effective catalysts with diverse morphologies for electrochemical ammonia synthesis.
研究领域:
电化学
·
催化
·
材料科学
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Ziyuan Xiu,Wei Mu,Xin Zhou,Xiaojun Han
The electrocatalytic N 2 reduction reaction (NRR) is expected to supersede the traditional Haber-Bosch technology for NH 3 production under ambient conditions. The activity and selectivity of electrochemical NRR are restricted to a strong polarized electric field induced by the catalyst, correct electron transfer direction, and electron tunneling distance between bare electrode and active sites. By coupling the chemical vapor deposition method with the poly(methyl methacylate)-transfer method, an ultrathin sandwich catalyst, i.e., Fe atoms (polarized electric field layer) sandwiched between ultrathin (within electron tunneling distance) BN (catalyst layer) and graphene film (conducting layer), is fabricated for electrocatalytic NRR. The sandwich catalyst not only controls the transfer of electrons to the BN surface in the correct direction under applied voltage but also suppresses hydrogen evolution reaction by constructing a neutral polarization electric field without metal exposure. The sandwich electrocatalyst NRR system achieve NH 3 yield of 8.9 μg h −1 cm −2 and Faradaic Efficiency of 21.7%. The N 2 adsorption, activation, and polarization electric field changes of three sandwich catalysts (BN-Fe-G, BN-Fe-BN, and G-Fe-G) during the electrocatalytic NRR are investigated by experiments and density functional theory simulations. Driven by applied voltage, the neutral polarized electric field induced by BN-Fe-G leads to the high activity of electrocatalytic NRR.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Yongheng Xiong,Yuting Li,Shipeng Wan,Yang Yu,Shule Zhang,Qin Zhong
Electrochemical reduction of NO to NH 3 (NORR) is an attractive approach to mildly realize NO removal and valuable NH 3 production. The electrolyte, as function as the NO absorbent, is crucial to apply electrochemical technology in practical de-NO engineering. In this paper, the ferrous chelate acted as the electrolyte for effective NO absorption in NORR based on the Brown-ring reaction. The rGO and Au/rGO catalysts served as cathodes to realize ferrous regeneration for continuous NO reduction. The results revealed that ferric chelate could be fully reduced at lower onset potential on rGO electrode. The Au/rGO catalyst exhibited excellent average yield and selectivity for NH 3 at − 0.1 V and pH = 6.32, (14.6 μmol* h −1 * cm −2 and 65.2%, respectively). The Faradaic Efficiency of NH 3 could reach 98.3% at pH = 1.0. This work provides a valuable reference for effective NO adsorption and sustainable NO-to-NH 3 conversion.
研究领域:
环境科学
·
电化学工程
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Jiaxin Li,Dandan Wang,Renquan Guan,Yujun Zhang,Zhao Zhao,Hongju Zhai,Zaicheng Sun
Photocatalysis provides a sustainable route to convert N2 to NH3 with the aid of a photogenerated electron. Beyond the typical issue in the photocatalytic field, NH3 synthesis requires adsorption, activation, and hydrogenation of N2. In this report, Ni-doped TiO2 (Ni-x-TiO2) photocatalysts were fabricated by a simple sol–gel method to introduce the oxygen defects and Ni site on TiO2. The oxygen vacancy (Vo) enhances the adsorption of N2 on the catalyst surface. The Ni doping induced a defect energy level below the conduction band, which prefers to accept the photogenerated electron. The electron captured by Vo tends to transfer to the adsorbed N2 and activate N2. On the other hand, the Ni site is a typical H2 production site. It provides enough H2 for the hydrogenation of N2 to form NH3. To sum up all of these advantages, Ni-doped TiO2 displays a high NH3 production rate of 46.80 μmol·g–1·h–1 which is about 7 times higher than that of pure TiO2. This manuscript provides a potential method to design a highly efficient photocatalyst for the NH3 synthesis.
研究领域:
材料科学
·
催化
·
化学工程
·
环境科学
✓ 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）