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1.
Lin Jia Hui Yang Jun Deng Junmei Chen Yuan Zhou Pan Ding Leigang Li Na Han Yanguang Li 《中国化学》2019,37(5):497-500
Electrocatalytic carbon dioxide reduction holds great promise for reducing the atmospheric CO2 level and alleviating the energy crisis. High‐performance electrocatalysts are often required in order to lower the high overpotential and expedite the sluggish reaction kinetics of CO2 electroreduction. Copper is a promising candidate metal. However, it usually suffers from the issues of poor stability and low product selectivity. In this work, bimetallic Cu‐Bi is obtained by reducing the microspherical copper bismuthate (CuBi2O4) for selectively catalyzing the CO2 reduction to formate (HCOO–). The bimetallic Cu‐Bi electrocatalyst exhibits high activity and selectivity with the Faradic efficiency over 90% in a wide potential window. A maximum Faradaic efficiency of ~95% is obtained at –0.93 V versus reversible hydrogen electrode. Furthermore, the catalyst shows high stability over 6 h with Faradaic efficiency of ~95%. This study provides an important clue in designing new functional materials for CO2 electroreduction with high activity and selectivity. 相似文献
2.
Prof. Kazuya Nakata Takuya Ozaki Prof. Chiaki Terashima Prof. Akira Fujishima Prof. Yasuaki Einaga 《Angewandte Chemie (International ed. in English)》2014,53(3):871-874
The catalytic, electrocatalytic, or photocatalytic conversion of CO2 into useful chemicals in high yield for industrial applications has so far proven difficult. Herein, we present our work on the electrochemical reduction of CO2 in seawater using a boron‐doped diamond (BDD) electrode under ambient conditions to produce formaldehyde. This method overcomes the usual limitation of the low yield of higher‐order products, and also reduces the generation of H2. In comparison with other electrode materials, BDD electrodes have a wide potential window and high electrochemical stability, and, moreover, exhibit very high Faradaic efficiency (74 %) for the production of formaldehyde, using either methanol, aqueous NaCl, or seawater as the electrolyte. The high Faradaic efficiency is attributed to the sp3‐bonded carbon of the BDD. Our results have wide ranging implications for the efficient and cost‐effective conversion of CO2. 相似文献
3.
Xiaofu Sun Chunjun Chen Shoujie Liu Song Hong Qinggong Zhu Qingli Qian Buxing Han Jing Zhang Lirong Zheng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(14):4717-4721
Electrochemical reduction of CO2 into energy‐dense chemical feedstock and fuels provides an attractive pathway to sustainable energy storage and artificial carbon cycle. Herein, we report the first work to use atomic Ir electrocatalyst for CO2 reduction. By using α‐Co(OH)2 as the support, the faradaic efficiency of CO could reach 97.6 % with a turnover frequency (TOF) of 38290 h?1 in aqueous electrolyte, which is the highest TOF up to date. The electrochemical active area is 23.4‐times higher than Ir nanoparticles (2 nm), which is highly conductive and favors electron transfer from CO2 to its radical anion (CO2.?). Moreover, the more efficient stabilization of CO2.? intermediate and easy charge transfer makes the atomic Ir electrocatalyst facilitate CO production. Hence, α‐Co(OH)2‐supported atomic Ir electrocatalysts show enhanced CO2 activity and stability. 相似文献
4.
Subiao Liu Xue Feng Lu Jing Xiao Xin Wang Xiong Wen Lou 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(39):13966-13971
Bi2O3 nanosheets were grown on a conductive multiple channel carbon matrix (MCCM) for CO2RR. The obtained electrocatalyst shows a desirable partial current density of ca. 17.7 mA cm?2 at a moderate overpotential, and it is highly selective towards HCOOH formation with Faradaic efficiency approaching 90 % in a wide potential window and its maximum value of 93.8 % at ?1.256 V. It also exhibits a maximum energy efficiency of 55.3 % at an overpotential of 0.846 V and long‐term stability of 12 h with negligible degradation. The superior performance is attributed to the synergistic contribution of the interwoven MCCM and the hierarchical Bi2O3 nanosheets, where the MCCM provides an accelerated electron transfer, increased CO2 adsorption, and a high ratio of pyrrolic‐N and pyridinic‐N, while ultrathin Bi2O3 nanosheets offer abundant active sites, lowered contact resistance and work function as well as a shortened diffusion pathway for electrolyte. 相似文献
5.
Tianyu Zhang Xu Han Hongbin Yang Aijuan Han Enyuan Hu Yaping Li Xiao‐qing Yang Lei Wang Junfeng Liu Bin Liu 《Angewandte Chemie (International ed. in English)》2020,59(29):12055-12061
Single‐atom catalysts (SACs) show great promise for electrochemical CO2 reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single‐atom electrode greatly limit their performance. Herein, we prepared a nickel single‐atom electrode consisting of isolated, high‐density and low‐valent nickel(I) sites anchored on a self‐standing N‐doped carbon nanotube array with nickel–copper alloy encapsulation on a carbon‐fiber paper. The combination of single‐atom nickel(I) sites and self‐standing array structure gives rise to an excellent electrocatalytic CO2 reduction performance. The introduction of copper tunes the d‐band electron configuration and enhances the adsorption of hydrogen, which impedes the hydrogen evolution reaction. The single‐nickel‐atom electrode exhibits a specific current density of ?32.87 mA cm?2 and turnover frequency of 1962 h?1 at a mild overpotential of 620 mV for CO formation with 97 % Faradic efficiency. 相似文献
6.
Ao Yu Guoming Ma Jintian Jiang Yajing Hu Mingming Su Wangtao Long Shixin Gao Dr. Hsien-Yi Hsu Dr. Ping Peng Prof. Fang-Fang Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(40):10405-10412
Inspired by the spongy bone structures, three-dimensional (3D) sponge-like carbons with meso-microporous structures are synthesized through one-step electro-reduction of CO2 in molten carbonate Li2CO3−Na2CO3−K2CO3 at 580 °C. SPC4-0.5 (spongy porous carbon obtained by electrolysis of CO2 at 4 A for 0.5 h) is synthesized with the current efficiency of 96.9 %. SPC4-0.5 possesses large electrolyte ion accessible surface area, excellent wettability and electronical conductivity, ensuring the fast and effective mass and charge transfer, which make it an advcanced supercapacitor electrode material. SPC4-0.5 exhibits a specific capacitance as high as 373.7 F g−1 at 0.5 A g−1, excellent cycling stability (retaining 95.9 % of the initial capacitance after 10000 cycles at 10 A g−1), as well as high energy density. The applications of SPC4-0.5 in quasi-solid-state symmetric supercapacitor and all-solid-state flexible devices for energy storage and wearable piezoelectric sensor are investigated. Both devices show considerable capacitive performances. This work not only presents a controllable and facile synthetic route for the porous carbons but also provides a promising way for effective carbon reduction and green energy production. 相似文献
7.
Fei‐Yue Gao Shao‐Jin Hu Xiao‐Long Zhang Ya‐Rong Zheng Hui‐Juan Wang Zhuang‐Zhuang Niu Peng‐Peng Yang Rui‐Cheng Bao Tao Ma Zheng Dang Yong Guan Xu‐Sheng Zheng Xiao Zheng Jun‐Fa Zhu Min‐Rui Gao Shu‐Hong Yu 《Angewandte Chemie (International ed. in English)》2020,59(22):8706-8712
A considerable challenge in the conversion of carbon dioxide into useful fuels comes from the activation of CO2 to CO2.? or other intermediates, which often requires precious‐metal catalysts, high overpotentials, and/or electrolyte additives (e.g., ionic liquids). We report a microwave heating strategy for synthesizing a transition‐metal chalcogenide nanostructure that efficiently catalyzes CO2 electroreduction to carbon monoxide (CO). We found that the cadmium sulfide (CdS) nanoneedle arrays exhibit an unprecedented current density of 212 mA cm?2 with 95.5±4.0 % CO Faraday efficiency at ?1.2 V versus a reversible hydrogen electrode (RHE; without iR correction). Experimental and computational studies show that the high‐curvature CdS nanostructured catalyst has a pronounced proximity effect which gives rise to large electric field enhancement, which can concentrate alkali‐metal cations resulting in the enhanced CO2 electroreduction efficiency. 相似文献
8.
Jianyu Han Chang Long Jing Zhang Ke Hou Yi Yuan Dawei Wang Xiaofei Zhang Xueying Qiu Yanfei Zhu Yin Zhang Zhongjie Yang Shuhao Yan Zhiyong Tang 《Chemical science》2020,11(39):10698
Electrocatalytic synthesis of multicarbon (C2+) products from CO2 reduction suffers from poor selectivity and low energy efficiency. Herein, a facile oxidation–reduction cycling method is adopted to reconstruct the Cu electrode surface with the help of halide anions. The surface composed of entangled Cu nanowires with hierarchical pores is synthesized in the presence of I−, exhibiting a C2 faradaic efficiency (FE) of 80% at −1.09 V vs. RHE. A partial current density of 21 mA cm−2 is achieved with a C2 half-cell power conversion efficiency (PCE) of 39% on this electrode. Such high selective C2 production is found to mainly originate from CO intermediate enrichment inside hierarchical pores rather than the surface lattice effect of the Cu electrode.The Cu electrode surface is reconstructed by a halide anion assisted method for promoting CO2 reduction. 相似文献
9.
Electrochemical Reduction of Carbon Dioxide to Methanol on Hierarchical Pd/SnO2 Nanosheets with Abundant Pd–O–Sn Interfaces
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Wuyong Zhang Qing Qin Dr. Lei Dai Ruixuan Qin Dr. Xiaojing Zhao Xumao Chen Daohui Ou Dr. Jie Chen Dr. Tracy T Chuong Prof. Binghui Wu Prof. Nanfeng Zheng 《Angewandte Chemie (International ed. in English)》2018,57(30):9475-9479
Electrochemical conversion of CO2 into fuels using electricity generated from renewable sources helps to create an artificial carbon cycle. However, the low efficiency and poor stability hinder the practical use of most conventional electrocatalysts. In this work, a 2D hierarchical Pd/SnO2 structure, ultrathin Pd nanosheets partially capped by SnO2 nanoparticles, is designed to enable multi‐electron transfer for selective electroreduction of CO2 into CH3OH. Such a structure design not only enhances the adsorption of CO2 on SnO2, but also weakens the binding strength of CO on Pd due to the as‐built Pd–O–Sn interfaces, which is demonstrated to be critical to improve the electrocatalytic selectivity and stability of Pd catalysts. This work provides a new strategy to improve electrochemical performance of metal‐based catalysts by creating metal oxide interfaces for selective electroreduction of CO2. 相似文献
10.
Song Liu Hong Bin Yang Sung‐Fu Hung Jie Ding Weizheng Cai Linghui Liu Jiajian Gao Xuning Li Xinyi Ren Zhichong Kuang Yanqiang Huang Tao Zhang Bin Liu 《Angewandte Chemie (International ed. in English)》2020,59(2):798-803
Designing effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) is an appealing approach to tackling the challenges posed by rising CO2 levels and realizing a closed carbon cycle. However, fundamental understanding of the complicated CO2RR mechanism in CO2 electrocatalysis is still lacking because model systems are limited. We have designed a model nickel single‐atom catalyst (Ni SAC) with a uniform structure and well‐defined Ni‐N4 moiety on a conductive carbon support with which to explore the electrochemical CO2RR. Operando X‐ray absorption near‐edge structure spectroscopy, Raman spectroscopy, and near‐ambient X‐ray photoelectron spectroscopy, revealed that Ni+ in the Ni SAC was highly active for CO2 activation, and functioned as an authentic catalytically active site for the CO2RR. Furthermore, through combination with a kinetics study, the rate‐determining step of the CO2RR was determined to be *CO2?+H+→*COOH. This study tackles the four challenges faced by the CO2RR; namely, activity, selectivity, stability, and dynamics. 相似文献
11.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(31):9254-9258
The utilization of CO2 in Li‐CO2 batteries is attracting extensive attention. However, the poor rechargeability and low applied current density have remained the Achilles’ heel of this energy device. The gel polymer electrolyte (GPE), which is composed of a polymer matrix filled with tetraglyme‐based liquid electrolyte, was used to fabricate a rechargeable Li‐CO2 battery with a carbon nanotube‐based gas electrode. The discharge product of Li2CO3 formed in the GPE‐based Li‐CO2 battery exhibits a particle‐shaped morphology with poor crystallinity, which is different from the contiguous polymer‐like and crystalline discharge product in conventional Li‐CO2 battery using a liquid electrolyte. Accordingly, the GPE‐based battery shows much improved electrochemical performance. The achieved cycle life (60 cycles) and rate capability (maximum applied current density of 500 mA g−1) are much higher than most of previous reports, which points a new way to develop high‐performance Li‐CO2 batteries. 相似文献
12.
Hierarchical MoS2 Shells Supported on Carbon Spheres for Highly Reversible Lithium Storage
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Dr. Lei Zhang Prof. Xiong Wen Lou 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(18):5219-5223
Hierarchical MoS2 shells supported on carbon spheres (denoted as C@MoS2) have been synthesized through a one‐step hydrothermal method. The obtained hierarchical C@MoS2 microspheres simultaneously integrate the structural and compositional design rationales for high‐energy electrode materials based on two‐dimensional (2D) nanosheets. When evaluated as an anode material for lithium‐ion batteries (LIBs), the hierarchical C@MoS2 microspheres manifest high specific capacity, enhanced cycling stability and good rate capability. 相似文献
13.
G‐quadruplex Nanowires To Direct the Efficiency and Selectivity of Electrocatalytic CO2 Reduction
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Lei He Dr. Xiaofu Sun Prof. Hua Zhang Prof. Fangwei Shao 《Angewandte Chemie (International ed. in English)》2018,57(38):12453-12457
DNA as a medium for electron transfer has been widely used in photolytic processes but is seldom applied to dark reaction of CO2 reduction. A G‐quadruplex nanowire (tsGQwire) assembled by guanine tetranucleotides was used to host several metal complexes and further to mediate electron transfer processes in the electrochemical reduction of CO2 catalyzed by these complexes. The tsGQwire modified electrode increased the Faradaic efficiency of cobalt(II) phthalocyanine (CoIIPc) 2.5‐folds for CO production than bare CoIIPc electrode, with a total current density of 11.5 mA cm?2. Comparable Faradaic efficiency of HCOOH production was achieved on tsGQwire electrode when the catalytic center was switched to a GQ targeting Ru complex. The high efficiency and selectivity of electrocatalytic CO2 reduction was attributed to the unique binding of metal complexes on G‐quadruplex and electron transfer mediated by GQ nanowire to achieve efficient redox cycling of catalytic centers on the electrode. 相似文献
14.
Ratnadip De Sabrina Gonglach Shounik Paul Michael Haas S. S. Sreejith Philipp Gerschel Ulf‐Peter Apfel Thanh Huyen Vuong Jabor Rabeah Soumyajit Roy Wolfgang Schfberger 《Angewandte Chemie (International ed. in English)》2020,59(26):10527-10534
The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular MnIII‐corrole complex, which is modified on the three meso‐positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2. Electrochemical reduction of MnIII leads to an electroactive MnII species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h?1, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the MnIII‐corrole center. 相似文献
15.
Chenxia Kang Dr. Ju Fang Likang Fu Shuxian Li Prof. Qiming Liu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(69):16392-16401
A 3D hierarchical carbon cloth/nitrogen-doped carbon nanowires/Ni@MnO2 (CC/N-CNWs/Ni@MnO2) nanocomposite electrode was rationally designed and prepared by electrodeposition. The N-CNWs derived from polypyrrole (PPy) nanowires on the carbon cloth have an open framework structure, which greatly increases the contact area between the electrode and electrolyte and provides short diffusion paths. The incorporation of the Ni layer between the N-CNWs and MnO2 is beneficial for significantly enhancing the electrical conductivity and boosting fast charge transfer as well as improving the charge-collection capacity. Thus, the as-prepared 3D hierarchical CC/N-CNWs/Ni@MnO2 electrode exhibits a higher specific capacitance of 571.4 F g−1 compared with those of CC/N-CNWs@MnO2 (311 F g−1), CC/Ni@MnO2 (196.6 F g−1), and CC@MnO2 (186.1 F g−1) at 1 A g−1 and remarkable rate capability (367.5 F g−1 at 10 A g−1). Moreover, asymmetric supercapacitors constructed with CC/N-CNWs/Ni@MnO2 as cathode material and activated carbon as anode material deliver an impressive energy density of 36.4 W h kg−1 at a power density of 900 W kg−1 and a good cycling life (72.8 % capacitance retention after 3500 cycles). This study paves a low-cost and simple way to design a hierarchical nanocomposite electrode with large surface area and superior electrical conductivity, which has wide application prospects in high-performance supercapacitors. 相似文献
16.
Dr. Yunxiang Li Zhihao Pei Dr. Deyan Luan Prof. Dr. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2023,62(19):e202302128
Gas-liquid-solid triple-phase interfaces (TPI) are essential for promoting electrochemical CO2 reduction, but it remains challenging to maximize their efficiency while integrating other desirable properties conducive to electrocatalysis. Herein, we report the elaborate design and fabrication of a superhydrophobic, conductive, and hierarchical wire membrane in which core–shell CuO nanospheres, carbon nanotubes (CNT), and polytetrafluoroethylene (PTFE) are integrated into a wire structure (designated as CuO/F/C(w); F, PTFE; C, CNT; w, wire) to maximize their respective functions. The realized architecture allows almost all CuO nanospheres to be exposed with effective TPI and good contact to conductive CNT, thus increasing the local CO2 concentration on the CuO surface and enabling fast electron/mass transfer. As a result, the CuO/F/C(w) membrane attains a Faradaic efficiency of 56.8 % and a partial current density of 68.9 mA cm−2 for multicarbon products at −1.4 V (versus the reversible hydrogen electrode) in the H-type cell, far exceeding 10.1 % and 13.4 mA cm−2 for bare CuO. 相似文献
17.
Lingzhen Gong Yongping Hang Jinhao Li Gang Dai Agula Bao 《Surface and interface analysis : SIA》2022,54(8):899-908
Hierarchical porous carbons are widely used as adsorbents, catalyst supports, electrode materials, and other applications because of their high specific surface area (SSA), varied pore structure, adjustable porosity, and excellent physicochemical stability. Introducing heteroatoms such as N, P, or S, with electronegativities different from that of carbon, into the carbon skeleton can change the chemical properties of the surface and the density of the electron cloud around the carbon matrix, thus altering interactions of CO2molecules with the surface and improving CO2adsorption capacity. Therefore, doping heteroatoms in carbon materials has attracted a great amount of attention. In this paper, the template method was used with F108 (polyethylene glycol–polypropylene glycolpolyethylene glycol) as the template, resorcinol and formaldehyde solutions as the carbon sources, phosphoric acid as the phosphorus source, and KOH as the activator to prepare phosphorus-doped hierarchical porous carbons. Through a series of characterization and CO2adsorption experiments, the influence of the amount of KOH and template agent on the pore structure of carbon materials was studied. We conclude that these phosphorus-doped hierarchical porous carbon materials are promising CO2adsorbents. 相似文献
18.
Metal‐Free Fluorine‐Doped Carbon Electrocatalyst for CO2 Reduction Outcompeting Hydrogen Evolution
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Dr. Jiafang Xie Xiaotao Zhao Prof. Maoxiang Wu Prof. Qiaohong Li Prof. Yaobing Wang Prof. Jiannian Yao 《Angewandte Chemie (International ed. in English)》2018,57(31):9640-9644
The electrochemical CO2 reduction (ECDRR), as a key reaction in artificial photosynthesis to implement renewable energy conversion/storage, has been inhibited by the low efficiency and high costs of the electrocatalysts. Herein, we synthesize a fluorine‐doped carbon (FC) catalyst by pyrolyzing commercial BP 2000 with a fluorine source, enabling a highly selective CO2‐to‐CO conversion with a maximum Faradaic efficiency of 90 % at a low overpotential of 510 mV and a small Tafel slope of 81 mV dec?1, outcompeting current metal‐free catalysts. Moreover, the higher partial current density of CO and lower partial current density of H2 on FC relative to pristine carbon suggest an enhanced inherent activity towards ECDRR as well as a suppressed hydrogen evolution by fluorine doping. Fluorine doping activates the neighbor carbon atoms and facilitates the stabilization of the key intermediate COOH* on the fluorine‐doped carbon material, which are also blocked for competing hydrogen evolution, resulting in superior CO2‐to‐CO conversion. 相似文献
19.
Dr. Xiudong Zhang Dr. Xupeng Yan Dr. Peng Chen Dr. Pei Zhang Prof. Dr. Xinchen Kang Dr. Jun Ma Prof. Dr. Chunjun Chen Prof. Dr. Buxing Han 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2024,136(9):e202315822
Electroreduction of CO2 into valuable chemicals and fuels is a promising strategy to mitigate energy and environmental problems. However, it usually suffers from unsatisfactory selectivity for a single product and inadequate electrochemical stability. Herein, we report the first work to use cationic Gemini surfactants as modifiers to boost CO2 electroreduction to formate. The selectivity, activity and stability of the catalysts can be all significantly enhanced by Gemini surfactant modification. The Faradaic efficiency (FE) of formate could reach up to 96 %, and the energy efficiency (EE) could achieve 71 % over the Gemini surfactants modified Cu electrode. In addition, the Gemini surfactants modified commercial Bi2O3 nanosheets also showed an excellent catalytic performance, and the FE of formate reached 91 % with a current density of 510 mA cm−2 using the flow cell. Detailed studies demonstrated that the double quaternary ammonium cations and alkyl chains of the Gemini surfactants played a crucial role in boosting electroreduction CO2, which can not only stabilize the key intermediate HCOO* but also provide an easy access for CO2. These observations could shine light on the rational design of organic modifiers for promoted CO2 electroreduction. 相似文献
20.
Yijing Chen Peng Li Hyunho Noh Chung‐Wei Kung Cassandra T. Buru Xingjie Wang Xuan Zhang Omar K. Farha 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(23):7764-7768
The efficient fixation of excess CO2 from the atmosphere to yield value‐added chemicals remains crucial in response to the increasing levels of carbon emission. Coupling enzymatic reactions with electrochemical regeneration of cofactors is a promising technique for fixing CO2, while producing biomass which can be further transformed into biofuels. Herein, a bioelectrocatalytic system was established by depositing crystallites of a mesoporous metal–organic framework (MOF), termed NU‐1006, containing formate dehydrogenase, on a fluorine‐doped tin oxide glass electrode modified with Cp*Rh(2,2′‐bipyridyl‐5,5′‐dicarboxylic acid)Cl2 complex. This system converts CO2 into formic acid at a rate of 79±3.4 mm h?1 with electrochemical regeneration of the nicotinamide adenine dinucleotide cofactor. The MOF–enzyme composite exhibited significantly higher catalyst stability when subjected to non‐native conditions compared to the free enzyme, doubling the formic acid yield. 相似文献