Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,prim...Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,primarily involving the reaction between hydrogen(H_(2))and nitrogen(N_(2))at temperatures ranging from 400 to 500℃ and pressures exceeding 100 bar.A global total of 180 million metric tons of ammonia were produced annually in centralized industrial plants through the Haber-Bosch process,which consumes roughly 1% of the global energy supply and contributes over 1.3% of global carbon dioxide emissions[1].展开更多
In this paper,the etching characteristics of the ultra-high resistivity silicon（UHRS） by using the Bosch process were investigated.The experimental results indicated that the sulfur hexafluoride flux,the temperature...In this paper,the etching characteristics of the ultra-high resistivity silicon（UHRS） by using the Bosch process were investigated.The experimental results indicated that the sulfur hexafluoride flux,the temperature of the substrate,the platen power and the etching intermittence had important influence on the etching rate and the etching morphology of the UHRS.The profiles and morphologies of sidewall were characterized with scanning electron microscopy（SEM）.By using an improved three-stage Bosch process,380-μm deep through holes were fabricated on the UHRS with the average etching rate of about 3.14 μm/min.Meanwhile,the fabrication mechanism of deep through holes on the UHRS by using the three-stage Bosch process was illustrated on the basis of the experimental results.展开更多
Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)...Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)reduction reaction(NRR)offers us an environmentally-friendly and sustainable route for NH_(3)synthesis under ambient conditions.展开更多
The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,si...The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,since an efficient electrocatalyst is required to perform the N_(2) reduction reaction (NRR) at room temperature,N_(2) activation is a severe challenge.Herein,we report a CeP nanoparticle–reduced graphene oxide (CeP–rGO) hybrid as an effective electrocatalyst for NH_(3) synthesis.In 0.1 M HCl,CeP–rGO achieves a large NH_(3) yield of 28.69 μg h^(−1) mg_(cat.)^(−1) and a high faradaic efficiency of 9.6% at −0.40 V,and it also shows high electrochemical and structural stability.Density functional theory (DFT) calculations show that CeP can efficiently catalyze the synthesis of NH_(3).展开更多
Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiF...Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiFe_(2)O_(4) nanosheet arrays on carbon cloth (NiFe_(2)O_(4)/CC) for high-efficiency NH_(3) electrosynthesis via the selective reduction of NO_(3)^(-) under ambient conditions. When operated in 0.1 M phosphate-buffered solution with additional 0.1 M NaNO_(3),such NiFe_(2)O_(4)/CC achieves a remarkable faradaic efficiency of 96.6% and a high NH_(3) yield of up to 10.3 mg h^(-1) cm^(-2). Furthermore,it possesses excellent electrochemical and structural stability. The theoretical calculations reveal that the metallic NiFe_(2)O_(4) surface has strong interactions with NO_(3)^(-) and can seriously inhibit the HER aiding in more efficient NO_(3)^(-) reduction to NH_(3).展开更多
Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carb...Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carbon neutralization.Electrochemical N_(2) reduction is regarded as a clean strategy to deal with this problem.In this work,porous LiFe_(5)O_(8) nanoparticle–reduced graphene oxide (rGO) is proposed as an efficient electrocatalyst for artificial N_(2)-to-NH_(3) fixation with excellent selectivity under ambient conditions.Electrochemical tests in 0.1 M HCl show that such a hybrid achieves a high NH_(3) yield of 36.025 mg h^(-1) mg_(cat.)^(-1) and a high faradaic efficiency of 13.08% at −0.2 V vs.the reversible hydrogen electrode.Furthermore,it also exhibits structural stability.Theoretical calculations reveal that LiFe_(5)O_(8)–rGO can efficiently catalyze NH_(3) synthesis with a low energy barrier.展开更多
As an environmentally friendly and sustainable method for ammonia synthesis,nitrogen reduction reaction(NRR)by electrocatalysis possesses several advantages,including viability under mild conditions,abundant reaction ...As an environmentally friendly and sustainable method for ammonia synthesis,nitrogen reduction reaction(NRR)by electrocatalysis possesses several advantages,including viability under mild conditions,abundant reaction raw materials and low energy consumption,and thus it is supposed to be a promising alternative to the traditional Haber-Bosch process.However,the stable NuN bonds in the nitrogen(N_(2))and the competing hydrogen evolution reaction(HER)put harsh requirements on catalysts.展开更多
The Haber-Bosch process for industrial-scale NH_(3)production suffers from harsh reaction conditions with CO_(2)emission.Electrochemical N_(2)reduction has gained considerable recent interest as an ecofriendly and sus...The Haber-Bosch process for industrial-scale NH_(3)production suffers from harsh reaction conditions with CO_(2)emission.Electrochemical N_(2)reduction has gained considerable recent interest as an ecofriendly and sustainable alternative for NH_(3)synthesis with the aid of efficient electrocatalysts for the N_(2)reduction reaction(NRR).Here,an Fe_(2)O_(3)nanoparticle-reduced graphene oxide composite(Fe_(2)O_(3)-rGO)is reported to be an Earth-abundant NRR electrocatalyst,enabling efficient ambient N_(2)-to-NH_(3)conversion.In 0.5 M LiClO_(4),this Fe_(2)O_(3)-rGO attains a large NH_(3)yield of 22.13μg h-1 mg^(-1)cat at-0.50 V and a high faradaic efficiency of 5.89%at-0.40 V(vs.RHE).It also demonstrates high electrochemical stability.展开更多
Electrochemical nitrogen reduction reaction(ENRR)under ambient conditions offers a greatly promising alternative to the highly-polluting Haber-Bosch process for the production of ammonia.However,due to their unsatisfa...Electrochemical nitrogen reduction reaction(ENRR)under ambient conditions offers a greatly promising alternative to the highly-polluting Haber-Bosch process for the production of ammonia.However,due to their unsatisfactory catalytic efficiency,and fussy and costly fabrication process,noble metal-based electrocatalysts can hardly promote the ammonia yield rate for industrial application efficiently.展开更多
The electrochemical nitrate reduction reaction(NtRR)under ambient conditions is regarded as a potential approach to achieve NH3 production,which currently heavily relies on the Haber–Bosch process at the cost of a hu...The electrochemical nitrate reduction reaction(NtRR)under ambient conditions is regarded as a potential approach to achieve NH3 production,which currently heavily relies on the Haber–Bosch process at the cost of a huge amount of energy and the massive production of CO_(2).Herein,a flower-like CuCo_(2)O_(4)spinel was synthesized via a two-step urea-assisted hydrothermal treatment and calcination process.展开更多
Electrocatalytic N_(2)reduction is a sustainable alternative to the Haber-Bosch process for ambient NH_(3)synthesis,but it needs efficient and stable catalysts.Herein,a hybrid of TiO_(2)and juncus effusus-derived carb...Electrocatalytic N_(2)reduction is a sustainable alternative to the Haber-Bosch process for ambient NH_(3)synthesis,but it needs efficient and stable catalysts.Herein,a hybrid of TiO_(2)and juncus effusus-derived carbon microtubes with a three-dimensional cross-linked hollow tubular structure is proposed as an efficient electrocatalyst for N_(2)-to-NH_(3)conversion at ambient conditions.In 0.1 M Na_(2)SO_(4),this catalyst offers a large NH_(3)yield of 20.03µg h^(-1)mg_(cat.)^(-1)and a high faradaic efficiency of 10.76%at-0.50 V versus the reversible hydrogen electrode,with superior electrochemical and structural stability.展开更多
基金supported by the National Natural Science Foundation of China(No.22105226)the Fundamental Research Funds for the Central Universities(23CX06019A and R20220132).
文摘Ammonia(NH_(3))is considered as one of the essential feedstocks in the fertilizer and chemical industries,serving as an ideal zero-carbon energy carrier.The ammonia synthesis process relies on Haber-Bosch process,primarily involving the reaction between hydrogen(H_(2))and nitrogen(N_(2))at temperatures ranging from 400 to 500℃ and pressures exceeding 100 bar.A global total of 180 million metric tons of ammonia were produced annually in centralized industrial plants through the Haber-Bosch process,which consumes roughly 1% of the global energy supply and contributes over 1.3% of global carbon dioxide emissions[1].
基金Project supported by the National Natural Science Foundation of China(Nos.61574108,61574112,61504099)
文摘In this paper,the etching characteristics of the ultra-high resistivity silicon（UHRS） by using the Bosch process were investigated.The experimental results indicated that the sulfur hexafluoride flux,the temperature of the substrate,the platen power and the etching intermittence had important influence on the etching rate and the etching morphology of the UHRS.The profiles and morphologies of sidewall were characterized with scanning electron microscopy（SEM）.By using an improved three-stage Bosch process,380-μm deep through holes were fabricated on the UHRS with the average etching rate of about 3.14 μm/min.Meanwhile,the fabrication mechanism of deep through holes on the UHRS by using the three-stage Bosch process was illustrated on the basis of the experimental results.
基金the National Key Research and Development Program of China(No.2017YFB0307504)the National Natural Science Foundation of China(No.21506133)the Youth Foundation of Sichuan University(No.2017SCU04a08)for their support in this research.
文摘Currently,the energy and capital intensive Haber–Bosch process still dominates NH_(3)synthesis which operates at high temperatures and pressures releasing inevitably large amounts of CO_(2).The electrocatalytic N_(2)reduction reaction(NRR)offers us an environmentally-friendly and sustainable route for NH_(3)synthesis under ambient conditions.
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘The Haber Bosch industrial NH_(3) production process has high energy consumption and severe CO_(2) emission.Electrochemical N_(2) reduction is an attractive method for the synthesis of carbon-neutral NH_(3).However,since an efficient electrocatalyst is required to perform the N_(2) reduction reaction (NRR) at room temperature,N_(2) activation is a severe challenge.Herein,we report a CeP nanoparticle–reduced graphene oxide (CeP–rGO) hybrid as an effective electrocatalyst for NH_(3) synthesis.In 0.1 M HCl,CeP–rGO achieves a large NH_(3) yield of 28.69 μg h^(−1) mg_(cat.)^(−1) and a high faradaic efficiency of 9.6% at −0.40 V,and it also shows high electrochemical and structural stability.Density functional theory (DFT) calculations show that CeP can efficiently catalyze the synthesis of NH_(3).
基金supported by the National Natural Science Foundation of China(No.22072015)。
文摘Ambient ammonia synthesis via the electrochemical reduction of nitrate (NO_(3)^(-)) offers us a sustainable alternative to the industrial energy-intensive Haber–Bosch process. Here,we report on the development of NiFe_(2)O_(4) nanosheet arrays on carbon cloth (NiFe_(2)O_(4)/CC) for high-efficiency NH_(3) electrosynthesis via the selective reduction of NO_(3)^(-) under ambient conditions. When operated in 0.1 M phosphate-buffered solution with additional 0.1 M NaNO_(3),such NiFe_(2)O_(4)/CC achieves a remarkable faradaic efficiency of 96.6% and a high NH_(3) yield of up to 10.3 mg h^(-1) cm^(-2). Furthermore,it possesses excellent electrochemical and structural stability. The theoretical calculations reveal that the metallic NiFe_(2)O_(4) surface has strong interactions with NO_(3)^(-) and can seriously inhibit the HER aiding in more efficient NO_(3)^(-) reduction to NH_(3).
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘Traditional NH_(3) production based on the Haber–Bosch process is usually accompanied by high energy consumption and a large amount of carbon dioxide emission,which are not conducive to the realization of global carbon neutralization.Electrochemical N_(2) reduction is regarded as a clean strategy to deal with this problem.In this work,porous LiFe_(5)O_(8) nanoparticle–reduced graphene oxide (rGO) is proposed as an efficient electrocatalyst for artificial N_(2)-to-NH_(3) fixation with excellent selectivity under ambient conditions.Electrochemical tests in 0.1 M HCl show that such a hybrid achieves a high NH_(3) yield of 36.025 mg h^(-1) mg_(cat.)^(-1) and a high faradaic efficiency of 13.08% at −0.2 V vs.the reversible hydrogen electrode.Furthermore,it also exhibits structural stability.Theoretical calculations reveal that LiFe_(5)O_(8)–rGO can efficiently catalyze NH_(3) synthesis with a low energy barrier.
基金supported by the National Natural Science Foundation of China(Grants 52072152,51802126)the Jiangsu University Jinshan Professor Fund,the Jiangsu Specially Appointed Professor Fund,Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation(2022M721372)+1 种基金“Doctor of Entrepreneurship and Innovation”in Jiangsu Province(JSSCBS20221197)Opening Fund of China National Textile and Apparel Council Key Laboratory of Flexible Devices for Intelligent Textile Apparel,Soochow University(SDHY2228).
文摘As an environmentally friendly and sustainable method for ammonia synthesis,nitrogen reduction reaction(NRR)by electrocatalysis possesses several advantages,including viability under mild conditions,abundant reaction raw materials and low energy consumption,and thus it is supposed to be a promising alternative to the traditional Haber-Bosch process.However,the stable NuN bonds in the nitrogen(N_(2))and the competing hydrogen evolution reaction(HER)put harsh requirements on catalysts.
基金supported by the National Natural Science Foundation of China(No.21575137).
文摘The Haber-Bosch process for industrial-scale NH_(3)production suffers from harsh reaction conditions with CO_(2)emission.Electrochemical N_(2)reduction has gained considerable recent interest as an ecofriendly and sustainable alternative for NH_(3)synthesis with the aid of efficient electrocatalysts for the N_(2)reduction reaction(NRR).Here,an Fe_(2)O_(3)nanoparticle-reduced graphene oxide composite(Fe_(2)O_(3)-rGO)is reported to be an Earth-abundant NRR electrocatalyst,enabling efficient ambient N_(2)-to-NH_(3)conversion.In 0.5 M LiClO_(4),this Fe_(2)O_(3)-rGO attains a large NH_(3)yield of 22.13μg h-1 mg^(-1)cat at-0.50 V and a high faradaic efficiency of 5.89%at-0.40 V(vs.RHE).It also demonstrates high electrochemical stability.
基金supported by the funding from Tianjin Natural Science Foundation(19JCQNJC05000)National Natural Science Foundation of China(Grant No.22005220).
文摘Electrochemical nitrogen reduction reaction(ENRR)under ambient conditions offers a greatly promising alternative to the highly-polluting Haber-Bosch process for the production of ammonia.However,due to their unsatisfactory catalytic efficiency,and fussy and costly fabrication process,noble metal-based electrocatalysts can hardly promote the ammonia yield rate for industrial application efficiently.
基金financially supported by the Natural Science Foundation of Anhui Province(Grant No.2108085QB60 and 2108085QB61)the CASHIPS Director's Fund(Grant No.YZJJ2021QN18 and YZJJ2021QN21)+1 种基金the China Postdoctoral Science Foundation(Grant No.2020M682057)the CAS/SAFEAInternational Partnership Program for Creative Research Teams of Chinese Academy of Sciences,China.
文摘The electrochemical nitrate reduction reaction(NtRR)under ambient conditions is regarded as a potential approach to achieve NH3 production,which currently heavily relies on the Haber–Bosch process at the cost of a huge amount of energy and the massive production of CO_(2).Herein,a flower-like CuCo_(2)O_(4)spinel was synthesized via a two-step urea-assisted hydrothermal treatment and calcination process.
基金supported by the National Natural Science Foundation of China(No.22072015).
文摘Electrocatalytic N_(2)reduction is a sustainable alternative to the Haber-Bosch process for ambient NH_(3)synthesis,but it needs efficient and stable catalysts.Herein,a hybrid of TiO_(2)and juncus effusus-derived carbon microtubes with a three-dimensional cross-linked hollow tubular structure is proposed as an efficient electrocatalyst for N_(2)-to-NH_(3)conversion at ambient conditions.In 0.1 M Na_(2)SO_(4),this catalyst offers a large NH_(3)yield of 20.03µg h^(-1)mg_(cat.)^(-1)and a high faradaic efficiency of 10.76%at-0.50 V versus the reversible hydrogen electrode,with superior electrochemical and structural stability.
