Article
Chemistry, Physical
Yuanzheng Zhang, Xiang Chen, Weilai Wang, Lifeng Yin, John C. Crittenden
Summary: This study designed and prepared Au1Cu (111) single-atom alloys with superior performance for electrocatalytic reduction of nitrate to ammonia in wastewater. The Au1Cu catalyst showed high NH3 production rate and Faradaic efficiency, and exhibited excellent durability without significant activity decay. Furthermore, the produced ammonia can be easily recovered through membrane distillation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Multidisciplinary
Xingchuan Li, Peng Shen, Yaojing Luo, Yunhe Li, Yali Guo, Hu Zhang, Ke Chu
Summary: In this study, PdFe1 single-atom alloy is developed as an effective electrocatalyst for nitrogen reduction reaction (NRR). Mechanistic investigations reveal that Pd-coordinated Fe single atoms serve as active centers, enabling efficient N-2 activation and exhibiting high selectivity and stability for the NRR.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Physical
Huimin Wang, Jingjing Huang, Jinmeng Cai, Yingying Wei, Ang Cao, Baozhong Liu, Siyu Lu
Summary: With the development of industrial and agricultural activities, the excessive production of nitrate has become a serious environmental and public health concern. Among various nitrate treatment techniques, electrochemical nitrate reduction reaction (eNRR) has gained significant attention due to its mild conditions and pollution-free nature. However, understanding the eNRR mechanism requires the use of in situ and operando techniques to study the reaction process at a time-resolved and atomic level.
Article
Chemistry, Physical
Patricia Poths, Anastassia N. Alexandrova
Summary: Improvements in operando spectroscopy have allowed for detailed investigation of the dynamic nature of catalysts under operating conditions. However, the high dynamicity of some catalysts presents a challenge, as they contain various thermally accessible states. Different techniques in catalysis research, such as ensemble-based and localized techniques, can provide insights into the dynamics of catalysts.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Review
Chemistry, Multidisciplinary
Wei Chen, Xianfeng Yi, Zhiqiang Liu, Xiaomin Tang, Anmin Zheng
Summary: This paper reviews the stabilization of carbocations in zeolites and summarizes advanced characterization methods for capturing carbocations. It clarifies the relationship between the activity and stability of carbocations in zeolite-catalyzed reactions.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Wanqiang Yu, Jiayuan Yu, Man Huang, Yujie Wang, Yijie Wang, Jiawei Li, Hong Liu, Weijia Zhou
Summary: CuNi alloy nanoparticles were synthesized on a Cu foil by laser irradiation for efficient electrocatalytic reduction of nitrate into ammonia. The synthesized CuNi NPs showed high performance and stability, and were used to construct a high-power density Zn-nitrate battery.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Xuanhao Wu, Mohammadreza Nazemi, Srishti Gupta, Adam Chismar, Kiheon Hong, Hunter Jacobs, Wenqing Zhang, Kali Rigby, Tayler Hedtke, Qingxiao Wang, Eli Stavitski, Michael S. Wong, Christopher Muhich, Jae-Hong Kim
Summary: The occurrence of high concentrations of nitrate in water resources poses a significant environmental and human health threat. Single atom alloys (SAAs) have shown promise in removing nitrate through thermocatalytic and electrocatalytic processes. This study reveals the contrasting performance of SAAs in thermocatalytic (T-NRR) and electrocatalytic (E-NRR) pathways, with Pd/Cu(1:100) SAA demonstrating the highest activity and selectivity for E-NRR. DFT calculations suggest that the superior performance of Pd/Cu(1:100) in E-NRR is attributed to the stability of NO3* in electrocatalysis and lower N2 formation barrier.
Article
Chemistry, Physical
Qinan Song, Miao Li, Xiaoshu Hou, Jiacheng Li, Zijun Dong, Shuo Zhang, Lei Yang, Xiang Liu
Summary: In this study, a single-atom iron electrode was synthesized and demonstrated for efficient nitrate reduction reaction. The catalyst achieved the highest nitrate removal capacity and a high faradaic efficiency. The designed pathway combined with electrochlorination allowed for complete conversion of byproducts to harmless nitrogen gas. This work offers a new paradigm for the development of nitrate removal from water bodies.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Qinan Song, Miao Li, Xiaoshu Hou, Jiacheng Li, Zijun Dong, Shuo Zhang, Lei Yang, Xiang Liu
Summary: This study synthesized a single-atom iron electrode for efficient NO3--N removal, demonstrating a new design paradigm and combining electrochlorination technology to convert by-products into harmless nitrogen gas.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Jinmeng Cai, Yingying Wei, Ang Cao, Jingjing Huang, Zheng Jiang, Siyu Lu, Shuang-Quan Zang
Summary: Converting nitrate to ammonia using electricity produced from renewable energy offers an alternative and sustainable approach for ammonia synthesis. This study presents a single-atom Ni-alloyed Cu catalyst that selectively converts nitrate into ammonia with a maximum Faradaic efficiency of around 100% and a yield rate of 326.7 mu mol h(-1) cm(-2) at 0.55 V versus reversible hydrogen electrode.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Engineering, Environmental
Yinghao Xue, Qihui Yu, Qian Ma, Yanyan Chen, Chuning Zhang, Wei Teng, Jianwei Fan, Wei-xian Zhang
Summary: Selective nitrate reduction and ammonia synthesis can be achieved at ambient conditions using atomic Cu sites anchored on micro-/mesoporous nitrogen-doped carbon, providing a potential solution for decentralized nitrate removal and utilization of nitrate-containing wastewater.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Physical
Shuo Wang, Lei Li, Kwan San Hui, Duc Anh Dinh, Zhiyi Lu, Qiuju Zhang, Kwun Nam Hui
Summary: Electrochemical nitrate reduction reaction (NO3RR) has potential in wastewater management and carbon-neutral ammonia synthesis, but lacks high-quality catalysts with controllable reaction pathways and high activity and selectivity. In this study, we explore the application of single atom alloys (SAAs) in nitrate reduction through high-throughput first-principles calculations. We identify Ni/Cu(111) as the most active SAA catalyst for NO3RR and find that the adsorption free energy of *NO3 can serve as an efficient descriptor to design and predict the NO3RR performance of SAAs. Furthermore, we reveal the pH-dependent properties of Cu-based SAAs, which influence the competition between the hydrogen evolution reaction (HER) and NO3RR.
Article
Chemistry, Physical
Faisal Rehman, Soonho Kwon, Charles B. Musgrave, Mohsen Tamtaji, William A. Goddard, Zhengtang Luo
Summary: This study systematically investigated the catalytic performance of metal-based dual-atom catalysts (DACs) anchored on two-dimensional expanded phthalocyanine (Pc) for electrocatalytic nitrate reduction to ammonia (NO3RR). The results showed that Cr2-Pc, V2-Pc, Ti2-Pc, and Mn2-Pc surfaces can efficiently produce ammonia with low limiting potentials. Moreover, the hydrogen evolution reaction is significantly suppressed on the DAC surface due to an ensemble effect.
Article
Chemistry, Physical
T. Len, P. Afanasiev, Y. Yan, M. Aouine, F. Morfin, L. Piccolo
Summary: The conversion of CO2 to methanol is an important process for environmental and energy transitions. This study investigates the performance of Mo-doped rutile titania nanorods as catalysts for methanol synthesis. It is found that these catalysts exhibit higher activity and selectivity compared to other forms of Mo catalysts. The study also reveals that the presence of rutile structure and single Mo atoms on the surface of the nanorods contribute to the enhanced performance.
Review
Chemistry, Multidisciplinary
Yuxiao Meng, Hongjie Huang, You Zhang, Yongyong Cao, Hanfeng Lu, Xi Li
Summary: Excess of carbon dioxide (CO2) in the atmosphere poses a significant threat to the global climate. The electrocatalytic carbon dioxide reduction reaction (CO2RR) is important for reducing environmental burden and exploring new energy sources. Single-atom catalysts (SACs) and double-atom catalysts (DACs) have been widely studied in electrocatalysis due to their high activity and selectivity. This review summarizes the research progress of electrocatalytic CO2RR using SACs and DACs, focusing on the reaction mechanism and the influence of solvation and electrode potential.
FRONTIERS IN CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Guike Zhang, Xiaotian Li, Kai Chen, Yali Guo, Dongwei Ma, Ke Chu
Summary: We have demonstrated the strong suitability of MBenes as a new type of tandem catalysts for electrocatalytic nitrate reduction to ammonia (NO3RR). FeB2 is employed as a model MBene catalyst for NO3RR, showing an impressive maximum NH3-Faradaic efficiency of 96.8% and a corresponding NH3 yield of 25.5 mg h(-1) cm(-2) at -0.6 V vs. RHE. Mechanistic studies reveal that the outstanding NO3RR activity of FeB2 arises from the tandem catalysis mechanism, where B sites activate NO3- to form intermediates, and Fe sites dissociate H2O and increase *H supply on B sites to enhance the intermediate hydrogenation and promote the conversion of NO3- to NH3.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Xiaotian Li, Kai Chen, Xubin Lu, Dongwei Ma, Ke Chu
Summary: This study presents the design of atomically dispersed Co anchored on MoS2 as a highly active and durable catalyst for electrocatalytic NO reduction to NH3. The Co1/MoS2 catalyst exhibits excellent NORR performance, outperforming most reported catalysts.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Ke Chu, Kai Chen, Peng Shen, Nana Zhang, Dongwei Ma
Summary: This study first reports that Mo2C is an active and selective NORR catalyst, and the surface-terminated Mo atoms on Mo2C can effectively activate NO, promote protonation energetics, and suppress proton adsorption, resulting in Mo2C's high NORR activity and selectivity.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Peng Shen, Guohui Wang, Kai Chen, Jilong Kang, Dongwei Ma, Ke Chu
Summary: The study demonstrates that Se-vacancy-rich WSe2 nanoplatelets are highly efficient catalysts for electrocatalytic nitrate reduction to ammonia (NO3RR). The introduction of Se-vacancy activates nitrate and reduces the reaction barriers, promoting the nitrate reduction process.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Physical
Yaojing Luo, Kai Chen, Peng Shen, Xingchuan Li, Xiaotian Li, Yunhe Li, Ke Chu
Summary: B-doped MoS2 nanosheet arrays are reported as efficient catalysts for NO3RR, achieving a NH3-Faradaic efficiency of 92.3% and a NH3 yield of 10.8 mg h-1 cm(-2) at -0.7 V (RHE). Theoretical calculations identify B-dopants as crucial active sites for enhancing NO3- activation and optimizing the free energies of reaction intermediates, resulting in enhanced NO3RR activity. Furthermore, B-MoS2 effectively suppresses undesired hydrogen evolution and exhibits high NO3RR selectivity.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Physical
Kai Chen, Ying Zhang, Jiaqi Xiang, Xiaolin Zhao, Xingang Li, Ke Chu
Summary: In this study, p-block Sb and Bi single-atom catalysts were designed and showed high efficiency in electrocatalytic NO reduction to NH3, with great potential for commercial applications.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Kai Chen, Jiaxin Wang, Jilong Kang, Xubin Lu, Xiaolin Zhao, Ke Chu
Summary: In this study, atomically Fe-doped and S-vacancy-rich MoS2 (Fe1/MoS2_x) is designed as a highly efficient electrocatalyst for NO-to-NH3 conversion. The Fe1/MoS2_x catalyst exhibits a maximum NH3-Faradaic efficiency of 82.5% and NH3 yield of 288.2 mu mol h_ 1 cm_ 2 at _ 0.6 V vs. RHE.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Guohui Wang, Ying Zhang, Kai Chen, Yali Guo, Ke Chu
Summary: Palladium phosphides are efficient catalysts for electrocatalytic reduction of nitrate to ammonia (NRA). PdP2 nanoparticles on reduced graphene oxide exhibit a NH3 Faradaic efficiency of 98.2% and a NH3 yield rate of 7.6 mg h-1 cm-2 at -0.6 V (RHE). Theoretical calculations suggest that the PdP2 (011) surface activates and hydrogenates NO3- through a NOH pathway while inhibiting the competitive hydrogen evolution reaction.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Kai Chen, Jiaxin Wang, Hu Zhang, Dongwei Ma, Ke Chu
Summary: In this study, single-atom W confined in MoO3-x amorphous nanosheets (W1/MoO3-x) with W1-O5 motifs was designed as a highly active and durable NORR catalyst. The dual functions of W1-O5 motifs were revealed through theoretical and operando spectroscopic investigations, which are to facilitate the activation and protonation of NO molecules and promote H2O dissociation while suppressing *H dimerization. This resulted in a self-tandem NORR mechanism of W1/MoO3-x, greatly accelerating the protonation energetics of the NOto-NH3 pathway, and achieving the highest NH3-Faradaic efficiency and NH3 yield rate among reported NORR catalysts.
Article
Chemistry, Physical
Kai Chen, Guohui Wang, Yali Guo, Dongwei Ma, Ke Chu
Summary: Atomically dispersed Ir confined in amorphous MoO3 (Ir-1/a-MoO3) was designed as a high-efficiency catalyst for electrochemical reduction reaction of NO to NH3 (NORR). The single-site Ir-1-O-5 moieties in Ir-1/a-MoO3 can powerfully activate and hydrogenate NO with a near-zero energy barrier and exhibit a higher affinity to NO over H adatoms, leading to enhanced NORR activity and selectivity. Ir-1/a-MoO3 shows a maximum NH3 yield rate of 438.8 mu mol & BULL;h(-1)& BULL;cm(-2) and NH3-Faradaic efficiency of 93.2%, making it one of the most efficient NORR catalysts to date.
Article
Chemistry, Physical
Guike Zhang, Nana Zhang, Kai Chen, Xiaolin Zhao, Ke Chu
Summary: In this study, atomically Mo-doped SnO2-x with enriched O-vacancies (Mo-SnO2-x) was reported as a high-efficiency NO3RR catalyst, achieving the highest NH3-Faradaic efficiency of 95.5% and NH3 yield rate of 5.3 mg h-1 cm-2 at -0.7 V (RHE). Experimental and theoretical investigations revealed that the d-p coupled Mo-Sn pairs on Mo-SnO2-x can synergistically enhance electron transfer efficiency, activate NO3-, and reduce the protonation barrier of the rate-determining step (*NO & RARR; *NOH), thereby significantly improving the kinetics and energetics of NO3RR.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Ying Zhang, Jiaqi Xiang, Kai Chen, Yali Guo, Dongwei Ma, Ke Chu
Summary: We found that Pd metallene is a highly efficient catalyst for electrocatalytic reduction of NO to NH3 (NORR), achieving a maximum NO-to-NH3 faradaic efficiency of 89.6% and a corresponding NH3 yield rate of 112.5 & mu;mol h(-1) cm(-2) at -0.3 V in neutral media. Theoretical calculations revealed that NO can be effectively activated and hydrogenated on the hcp site of Pd through a mixed pathway with a low energy barrier.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Kai Chen, Nana Zhang, Fuzhou Wang, Jilong Kang, Ke Chu
Summary: Main-group metal elements have potential for high-performance NO to NH3 electrochemical reduction (NORR) catalysts, but this area remains unexplored. In this study, main-group In single atoms confined in an amorphous MoO3 substrate (In-1/a-MoO3) are investigated as efficient NORR catalysts, demonstrating a maximum NH3 yield of 242.6 mu mol h(-1) cm(-2) and NH3-faradaic efficiency of 92.8%. Further experiments and theoretical analysis reveal that single-site In atoms serve as dominant active centers, inhibiting hydrogen evolution and optimizing the hydrogenation energetics of the NO-to-NH3 pathway.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Inorganic & Nuclear
Guohui Wang, Peng Shen, Kai Chen, Yali Guo, Xiaolin Zhao, Ke Chu
Summary: We report the use of rare-earth La-doped VS2-x catalyst enriched with S-vacancies (La-VS2-x) for electrochemical nitrate reduction to ammonia (NO3RR), which exhibits a NH3-faradaic efficiency of 96.6% and a corresponding NH3 yield rate of 11.3 mg h(-1) cm(-2) at -0.6 V vs. RHE. Theoretical computations reveal that La-dopants and S-vacancies synergistically enhance NO3- activation, suppress hydrogen evolution, and lower energetic barriers, resulting in improved NO3RR activity and selectivity of La-VS2-x.
INORGANIC CHEMISTRY FRONTIERS
(2023)
